Advancing Commercialization of Nanocellulose: Critical ...

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Advancing Commercialization of Nanocellulose:

Critical Challenges Workshop Report

March 2020

A Workshop hosted by the Alliance for Pulp & Paper Technology Innovation in collaboration with the USDA Forest Service and the National Nanotechnology

Coordinating Office

May 7-8, 2019

USDA Patriot’s Plaza III 355 E St SW, Washington, DC

Acknowledgements

The Advancing Commercialization of Nanocellulose: Critical Challenges Workshop was hosted by the Alliance for Pulp & Paper Technology Innovation (APPTI) in collaboration with the USDA Forest Service and the National Nanotechnology Coordinating Office in support of the Sustainable Nanomanufacturing Signature Initiative.

Workshop preparation and planning was led by the APPTI Nanocellulose Team members with major support by APPTI members and partners including GranBio Technologies, SAPPI, International Paper, Domtar, the University of Maine and the USDA Forest Service. The workshop co-chairs were Kim Nelson-CTO of Nanocellulose Technology, GranBio and Colleen Walker-Director Process Development Center, University of Maine. The USDA provided space for the workshop

in Patriot’s Plaza III. The National Nanotechnology Coordinating Office assisted in planning for and facilitation of the workshop. See Appendix A for the Organizing Committee roster.

The principle writers of this report were David Turpin of APPTI and Kim Nelson of GranBio.

APPTI also wishes to acknowledge the contributions of the workshop participants, speakers, and session chairs representing industry, academia, and government. A full list of participants can be found in Appendix B.

The information in this document is meant to be distributed widely throughout the forest products and material science industries and the broader research community. The sponsors encourage reproduction and dissemination of the entire document, or portions thereof, with attribution and without changes.

Contents

Acknowledgements ......................................................................................................... 2

Executive Summary ........................................................................................................ 4

Introduction ..................................................................................................................... 6

Session I: Emergence of Nanocellulose in the Bioeconomy ........................................... 8

Global Commercialization Activities ............................................................................. 8

End-user needs and challenges .................................................................................. 9

Session II – Critical Challenges ..................................................................................... 11

A Review of Nanocellulose Drying and Dewatering ................................................... 11

A Review of Nanocellulose Compatibilization for Polymer/Resin Composites ........... 12

Session III: Opportunities .............................................................................................. 16

Priority RESEARCH NEEDS ......................................................................................... 19

Session IV & V: Researchers & Realizers ..................................................................... 22

Session VI: Making it Happen - R&D Projects to Address RESEARCH NEEDS .......... 22

Dewatering & Drying Project Plan – Techno-Economic Analysis .............................. 23

Dewatering & Drying Project Plan – Structure-Process-Property Relationships ........ 24

Dewatering & Drying Project Plan – Water/CN Interactions ...................................... 25

Dewatering & Drying Project Plan -- Redispersion .................................................... 27

Plastics Compatibilization Project Plan – Functionalizing with Silane ........................ 28

Plastics Compatibilization Project Plan – Functionalizing without Silane ................... 29

Plastics Compatibilization Project Plan – Killer Applications ...................................... 30

Path Forward ................................................................................................................. 31

Appendix A - Workshop Organizing Committee ............................................................ 32

Appendix B - Workshop Participants ............................................................................. 33

Appendix C - Workshop Agenda ................................................................................... 34

Appendix D - US Capabilities and Expertise ................................................................. 36

Appendix E - Rapid Fire Presentations ......................................................................... 47

Appendix F - References ............................................................................................... 49

Advancing Commercialization of Nanocellulose: of 51 Critical Challenges Workshop

Executive Summary

Cellulose, the most abundant organic polymer on Earth, has been utilized by humanity for millennia for vital functions including fuel and energy, transportation, clothing, shelter and communication. In the 1950’s, scientists discovered that the ultra-strong, light-weight submicroscopic crystalline regions of cellulose contained in cells of trees could be isolated as a new nanomaterial, commonly referred to as nanocellulose. Today, many companies throughout the world are focused on the large scale extraction of nanocellulose from the cells of trees and agricultural residues for use in more sustainable, higher performance materials. Nanocellulose has a variety of unique distinguishing properties—including high strength, high absorbency, low density, and self-assembly properties—that make it promising for an array of commercial applications. In addition, because of their feedstock’s abundance, they potentially could be sustainably and renewably produced in quantities of tens of millions of tons per year.1 Nanocellulose-enhanced products currently on the market include running shoes with improved durability and cushioning, cleaning and hygiene products, oil and gas drilling fluids, and paper-based packaging for liquids.

The Alliance for Pulp & Paper Technology Innovation (APPTI) is a non-profit corporation whose mission includes supporting development of technology platforms that enable new revenue streams from forest-based biomass. The APPTI Cellulosic Nanomaterials Team focuses on facilitating the development of pre-competitive knowledge and technologies to overcome impediments to more rapid commercialization of nanocellulose.

Impediments to commercialization of

nanocellulose have been extensively reported in the 2014 US Forest Service and National Nanotechnology Initiative report on Nanocellulose Commercialization (FS-NNI Nanocellulose Commercialization Report, 2014) and the 2016 APPTI Cellulosic

Material Research Roadmap (APPTI Technology Roadmaps).

The 2016 APPTI Roadmap also identifies pre-competitive research and development (R&D) PRIORITY AREAS that could have the greatest potential for advancing both the manufacture and use of cellulose nanomaterials. The R&D PRIORITY AREAS are:

Environment, health, and safety (EHS) considerations

Measurement and standards for manufacturing

Characterization of cellulose nanomaterials

Controlling interactions between water and cellulosic nanomaterials

Dewatering and drying

Management of interfacial properties for polymer composites

Since 2016, significant progress has been made addressing many of the critical challenges in these areas.

A dietary study funded by nanocellulose stakeholders, including APPTI member companies, shows that fibrillated cellulose raises no safety concerns when used as a food ingredient.2

Foster et al. published a comprehensive review that establishes detailed best practices, methods and techniques for characterizing Cellulosic Nanomaterial (CN) particle morphology, surface chemistry, surface charge, purity, crystallinity, rheological properties, mechanical properties, and toxicity for two distinct forms of CNs: cellulose nanocrystals (CNCs) and cellulose nanofibrils (CNFs).3

Shimadzu Corporation, an analytical and measurement instrument provider, released a comprehensive “Solutions for Cellulose Nanomaterials Application Notebook” which provides detailed analysis of key properties of nanocellulose and nanocellulose reinforced composites including optical transmittance, morphology, dispersibility,

https://www.fpl.fs.fed.us/documnts/pdf2014/usforestservice_nih_2014_cellulose_nano_workshop_report.pdf



https://www.appti.org/technology-roadmaps-downloads.html

https://www.appti.org/technology-roadmaps-downloads.html

Advancing Commercialization of Nanocellulose: Critical Challenges Workshop of 51

identification of surface functional groups, and mechanical testing.4

For the PRIORITY AREAS relating to nanocellulose drying and dewatering (including associated unique water interactions) and interfacial compatibilization with plastic composites, APPTI members recognize that significant KNOWLEDGE GAPS and challenges remain.

As such, APPTI’s “Advancing Commercialization of Nanocellulose: Critical Challenges Workshop”, held May 7-8, 2019 in Washington, D.C. focused on these remaining critical, high-impact R&D PRIORITY AREAS impacting commercialization of nanocellulose: dewatering and drying and compatibilization.

The two-day session was devoted to determining critical KNOWLEDGE GAPS and RESEARCH NEEDS which, if overcome, would have the greatest impact on accelerating widespread implementation and commercialization of nanocellulose materials and applications. The agenda for the workshop is provided in Appendix C.

A cornerstone of the workshop was presentation of two state-of-the-art literature reviews commissioned by APPTI that assess the current understanding of drying and dewatering and compatibilization of nanocellulose for use in polymers and identified critical KNOWLEDGE GAPS. Brainstorming sessions were conducted to prioritize RESEARCH NEEDS (specific technical issues and challenges that if solved would have the greatest impact on commercialization). Workshop participants then outlined R&D project plans to address the priority research needs. These plans defined the project objectives, outcomes, performance metrics, current state of technology and knowledge, and activities to be conducted over the life of the project to execute the project scope and meet the project objectives. The intention of the project plans was to inspire additional thinking about solutions and motivate

stakeholders to form collaborative teams to take action to address these research needs.

Another primary goal of the workshop was to build a tighter, broader network of nanocellulose stakeholders within the US, as part of APPTI’s mission to elevate nanocellulose research and commercialization efforts by connecting stakeholders and fostering new collaborations. The workshop included 5-minute flash presentations from thirty of our country’s nanocellulose researchers, producers, end-users, equipment suppliers, and funding agencies. To highlight the exceptional capabilities and expertise of our country’s nanocellulose community, Appendix D provides a catalogue of active US-based nanocellulose community members along with their area of focus, expertise and unique assets in the field.


Introduction

Development of nanocellulose-enhanced products is an active area of research, development and deployment (R&D&D) throughout the world at universities, government labs, and commercial entities. As an indicator of growing research activity, the number of global patents and published patent applications increased 600% between 2010 and 2015, to 350 per year. There are currently 15 companies producing nanocellulose (including microfibrilated cellulose, cellulose nanofibrils and cellulose nanocrystals) at the demonstration scale or larger.5 There are over 225 companies, Universities, and Research Institutions across 22 European Countries performing research and development with nanocellulose. In Japan, the Nanocellulose Forum is a consortium of 220 companies including Toyota Auto Body Co., Mitsubishi Motors Corp., Mitsui Chemicals Inc. and others. Over 50 organizations in the US are engaged in nanocellulose R&D&D activities.

Governments throughout the world have recognized the potential economic and societal benefits of nanocellulose and have made significant R&D investments. For example, the Japanese Government invests ~$38 million annually in nanocellulose production and product development as part of their Japan Revitalization Strategy. As such, most commercial products have launched from Japan in niche markets.

In the US, funding primarily by the US Department of Agriculture and the Department of Energy have focused on supporting the installation and optimization of demonstration-scale production facilities at the USDA Forest Product Laboratory, the University of Maine, and GranBio’s Thomaston Biorefinery. These demonstration plants have been instrumental in moving nanocellulose-applications development from lab scale to pilot and commercial scale by supplying sizable quantities of nanocellulose to end-users over a period of 5+ years. The availability of large quantities of material for

evaluation and product development, development of low cost nanocellulose production methods, and increasing consumer demand for sustainable, environmentally-friendly products have recently moved nanocellulose from an entirely “market push” scenario to significantly more “market pull”.

The United States is uniquely positioned to lead commercialization of nanocellulose-enabled products.

Our workers are among the most productive in the world.

We have the world’s best research universities and are a global leader in innovation.

And we have the trees, the world’s 4th largest reserve, which are harvested by certified, sustainable practices to support our large forest products industry.

We also have the infrastructure for harvesting and delivery of forest-based resources to industrial sites which has been utilized for over 200 years.

The creation of new materials, new products, and new industries leads to new jobs. US manufacturing jobs have decreased 30% over the last 40-50 years, but large scale sustainable manufacturing of nanocellulose can help ameliorate this trend. The Annual US market potential for nanocellulose is estimated by the USDA Forest Service to be 6.4 million metric tons across various application.1

As with all new materials and processes, there remain technical challenges for wide-spread adoption. The APPTI team’s mission is to overcome the pre-competitive knowledge gaps impeding more rapid commercialization of nanocellulose with a particular focus on the most impactful: drying and dewatering, and compatibilization with plastics.

Dewatering, or concentrating, nanocellulose slurries for more efficient shipping or use in


water-limited applications is inherently difficult because of the high water-holding capacity and high viscosity of these materials at low concentrations. Furthermore, many applications, such as plastics reinforcement, require a completely dry nanocellulose product that maintains the particles’ nano-scale morphology. Preventing irreversible agglomeration of high surface area cellulosic materials during dewatering and drying is challenging due to formation of strong hydrogen bonds between particles. New technologies are needed for scalable, economical preservation of discrete nanocellulose particle morphology during dewatering and drying for effective low-energy re-dispersion in aqueous systems and hydrophobic plastic resins.

Structure of the Report

The purpose of this report is to summarize the workshop results and present the major conclusions to inform and guide planning and investments aimed at expediting the commercialization of cellulose nanomaterials. The report is organized following the workshop agenda.

The next section (Workshop Session I) presents an overview of cellulose nanomaterials: the background, the potential of the materials, and the current state of technology and applications in the United States.

Session II – Critical Challenges, presents the challenges, and knowledge gaps in both focus areas that were identified in the state-of-the-art literature reviews.

In Session III: Opportunities, the participants expanded the knowledge gaps and research needs and prioritized the list in terms of impact and time to implement.

In Sessions IV & V: Researchers & Realizers, the event showcased US capabilities in nanocellulose production and application. The summary from this session is presented in Appendix D which provides a catalogue of active US-based nanocellulose community. In addition, more

than two dozen suppliers and users gave rapid-fire presentations of their capabilities which can be found in Appendix E. The workshop, and report, wraps up with the section outlining R&D Projects which could address the research needs.


Session I: Emergence of Nanocellulose in the Bioeconomy

This introductory session presented the benefits of nanocellulose to the bioeconomy and national interests, provided an overview of global commercialization activities, described nanocellulose end-user needs and challenges, and offered advice on overcoming the challenges inherent to innovation and commercialization.

US Agriculture Under-Secretary Jim Hubbard stressed the urgent importance of innovative and emerging technologies to expand our options for preventing the escalation of devastating forest fires. Some 80 million acres have been identified by the Forest Service as at-risk and new markets for wood-based materials are critical for keeping our forests healthy and free of hazardous fuels.

Alexander Friend, Deputy Chief of the US Forest Service discussed the Forest Service’s continued financial investment in developing US-based nanocellulose production capacity and stressed his organization’s commitment to nanocellulose towards its mission “to sustain the health, diversity, and productivity of the Nation’s forests and grasslands to meet the needs of present and future generations.”

Lisa Friedersdorf, Director of the National Nanotechnology Coordination Office, discussed nanocellulose’s role in the Signature Initiative of the US’s National Nanotechnology Initiative. The NNI is a US Government research and development (R&D) initiative involving 20 departments and independent agencies working together towards advancing nanotechnology to benefit industry and society. The goal of the “Nanotechnology Signature Initiative - Sustainable Nanomanufacturing – Creating the Industries of the Future” is to accelerate the development of industrial-scale methods for manufacturing functional nanoscale systems. The initiative targets production-worthy scaling of three classes of sustainable materials (high-performance

structural carbon-based nanomaterials, optical metamaterials, and cellulosic nanomaterials) that have the potential to affect multiple industry sectors with significant economic impact.

Global Commercialization Activities

Jack Miller, Principle Consultant at Biobased Markets, presented progress in global commercialization of nanocellulose.

There are currently 15 companies producing nanocellulose (including microfibrilated cellulose, cellulose nanofibrils and cellulose nanocrystals) at the demonstration scale or larger.6

Nanocellulose Producers at Demonstration Scale or

Larger

(tonnes per year, dry basis)

Producer Material Capacity

FiberLean Technologies, UK MFC 8,800

Kruger, Canada CF 6,000

Borregaard, Norway MFC 1,100

Nippon Paper, Japan CNF 560

CelluForce, Canada CNC 300

Norske Skog, Norway MFC 260

University of Maine, USA CNF 260

Daicel, Japan MFC 200

RISE, transportable container

factory

MFC 200

GranBio Technologies, USA CNC 130

GranBio Technologies, USA CNF 130

CelluComp, UK CNF 100

Chuetsu Pulp and Paper, Japan CNF 100

International Paper MFC *

Stora Enso MFC *

* International Paper and Stora Enso are also reported to be producing MFC, largely for use in their own paper and paperboard. The 2017 Stora Enso Annual Report says "Stora Enso invested €9 million in new MFC production at Imatra, Ingerois and Fors mills. The new capacity corresponds to 500 000 tonnes of board made with MFC after a ramp-up period of 3–5 years."


Equity investment in companies producing nanocellulose continues:

CelluForce: investment from Schlumberger and Fibria (now Suzano) in addition to initial funding from Domtar and FPInnovations

American Process Inc.: acquisition by GranBio

FiberLean Technologies: launched as a joint venture by Omya and Imerys

Melodea: investment from Klabin and Holmen

In a 2019 market study, Biobased Markets estimated that in 2018 the global production of nanocellulose was 40,000 tonnes and is projected to grow at 30% per year. While the majority of this is associated with paper and paperboard mills producing microfibrillated cellulose (MFC) and using it in their own products, other applications are beginning to grow and close the gap.

Cellulose Nanomaterials Forecast to 2025

(tonnes)

2018 2020 2025 CAGR

Total 39,600 80,000 251,000 30%

Mills 30,000 45,000 125,000 23%

A number of on-the-market commercial applications outside of paper and paperboard have been reported, including oil and gas drilling fluids, adult diapers, coatings, composites, rubber latex, cosmetics, gel inks for pens, and foams for running shoes.

According to TAPPI’s 2018 book, Nanocellulose Challenges and Opportunities, End User Perspectives, three key drivers for expanding the nanocellulose market were identified by potential end-user companies: get the cost down, develop the value proposition through the supply chain, and collaborate.7

Getting the cost down is dependent on getting volumes up and achieving economies of scale, and to do this we need to develop the value propositions and

collaborate. The industry is doing just that. Leading producers have reported collaborations, joint development agreements, and supply agreements. GranBio Technologies has a Joint Development Agreement with Birla Carbon, the world’s largest carbon black producer, for low rolling resistance tires containing nanocellulose8. Borregaard participates in multiple consortia funded by the Bio-Based Industries Joint Undertaking (BBI JU), a public-private partnership between the European Union and the Bio-based Industries Consortium, for development of nanocellulose end-use applications.9 Imerys has signed two separate commercial agreements for the full-scale supply of FiberLean® MFC, with two leading papermakers, one in Asia and one in the USA.10

End-user needs and challenges

Workshop co-leads Kim Nelson of GranBio and Colleen Walker, University of Maine Product Development Center described end-user commercial needs. GranBio has been engaged in Joint Development Agreements with 10+ companies since 2015 to develop nanocellulose-enhanced commercial products across a variety of fields including tires and rubber goods, paperboard, adhesives, sealants, and plastic composites. Since 2013, the University of Maine has distributed samples of cellulose nanofibrils and cellulose nanocrystals to 305 companies, 276 universities, and 49 government and other entities. Dr. Nelson stressed that end-users in the plastic and rubber composites fields require nanocellulose in a masterbatch form for drop-in, dust-free dosing and handling.. For aqueous-based applications, end-users require concentrated nanocellulose with as high a solids content as possible, while being rapidly re-dispersible with low energy/standard mixing equipment. Dr. Walker reports that interactions between University of Maine and end-users are predominantly in paper applications. They have completed 11 Commercial scale trials and 3 high speed pilot trials with ~25 tons of


cellulose nanofibrils. Industries outside of the forest products / paper field require more help and engagement understanding these unique materials. She also stressed that it takes time (typically years) for new materials to be tested and incorporated into existing processes and products.

Michael Goergen, VP Innovation, US Endowment for Forestry and Communities and Director, P3 Nano, described P3 Nano’s accomplishments in advancing the demonstration and scale-up of innovative nanocellulose technologies that enhance the performance of concrete, including three field applications around the nation: a sidewalk in Madison, WI; a county bridge deck in northern California, and, the largest commercial test in the world, the Endowment’s parking lot in downtown Greenville, South Carolina11. P3Nano is a public-private partnership founded by the US Endowment and the USDA Forest Service aimed at rapidly commercializing cellulosic nanomaterials. With their partners, the Endowment is investing in non-competitive research to take full advantage of the unique properties of cellulose at the nanoscale. Based on the Endowment’s long history of supporting innovation, Mr. Goergen recognized the many challenges associated with commercializing innovative products, but stressed that the “valley of death” can be overcome through perseverance, financial commitment and relentless drive to launch sustainable materials that address global challenges.


Session II – Critical Challenges

APPTI’s Cellulose Nanomaterials Team identified two research and development (R&D) PRIORITY AREAS that have the greatest potential for advancing both the manufacture and use of cellulose nanomaterials: Dewatering and Drying and Compatibilization with Plastics. The team commissioned two current state-of-knowledge review papers in these areas to assess the current practices and technologies and remaining challenges or KNOWLEDGE GAPS.

A central goal of the workshop was to deconstruct the identified KNOWLEDGE GAPS into RESEARCH NEEDS, or specific technical issues and challenges that, if solved, would have the greatest impact on closing the KNOWLEDGE GAPS and lead to breakthroughs or new technology solutions to advance nanocellulose commercialization.

Another goal of the workshop was to frame actionable R&D approaches to address the RESEARCH NEEDS.

Greg Schueneman (US Forest Service) and Scott Sinquefield (Renewable Bioproducts Institute, Georgia Tech), presented their literature reviews on compatibilization and drying & dewatering, respectively. The literature reviews, which will be submitted for publication, provided workshop participants with an understanding of the up-to-date, state of the science on these two PRIORITY AREAS. The authors also suggested KNOWLEDGE GAPS and RESEACH NEEDS in the respective areas to seed conversation in workshop breakout sessions which were intended to prioritize the KNOWLEDGE GAPS in terms of impact and implementation time.

A Review of Nanocellulose Drying and Dewatering 12

Challenges

Nanocellulose is produced in dilute aqueous suspensions. Because of their high surface area and high concentration of surface

hydroxyl groups, both Cellulose Nanocrystals (CNC) and Cellulose Nanofibrils (CNF) share similar challenges with regard to dewatering, drying, and redispersion. Their high surface area, hydrophilic nature, and high water holding capacity contribute to dilute suspensions having high thixotropic viscosities. CNF and CNC suspensions as low as 2-3 wt.% and 6-7 wt.% solids (respectively) exhibit gel-like behavior and are commonly referred to as such. Dewatering and drying Nanocellulose (NC) by conventional methods can lead to particle agglomeration and hydrogen bonding of the fibrils/crystals such that they do not redisperse upon rehydration. However, dewatering (concentrating) and drying of NC are advantageous processes because of the high transport costs of shipping dilute aqueous suspensions as well as end-use application requirements. Depending on the application, NC may require redispersion in water such that the unique and purposely engineered nanoscale properties are retained. Additionally, many promising applications of NC require redispersion in organic mediums (e.g. plastics); and it must be dispersed to maintain the nano-scale benefits.

Current State-of-Knowledge Summary

Currently, strategies used for NC

dewatering include centrifugation 13,

filtration14,15,16, shear stress–promoted

dewatering17,18,19,20, pressing21,22, and

solvent evaporation23.

After dewatering, a drying step is needed to bring NC to a fully dried state. Currently, there are four types of drying technologies for NC suspensions: oven drying/solvent evaporation24,25, spray drying26,27,28,29, freeze drying30,31, and supercritical CO2 drying32,33. Sometimes these are used in combination, e.g., spray freeze drying and supercritical CO2 spray drying34.

KNOWLEDGE GAPS

Processes for drying of NC such that it is completely redispersible in water have been developed for certain specific applications of


NC. While cost studies for the commercial scale have not been published, the successful examples seem to be costly (e.g. requiring an expensive additive that must be recovered and reused). This could be justified for a high value product. Techno-economic analyses will be needed in each case. There is also the issue of the dispersion additive possibly remaining sorbed to the fibril and whether or not that is acceptable for the end use of the NC.

Some techniques to aid in dewatering were found in the literature. It is not clear though, at what threshold solids content the NC-water mass can be completely redispersed without the need for special measures such as sonication, ultra-high shear mixing, or the use of additives. This threshold solids content would be useful information for techno-economic studies.

If a simple, low-cost solution exists, it has not been made public yet. New technology is often kept confidential rather than patented. A general techno-economic (TE) model would be helpful that includes variable costs and product valuations, or a set of example TE studies for various promising applications.

More technologies and processes are needed to achieve the holy grail of scalable, low-energy, cost-effective preservation of NC fibril properties during drying for re-dispersion in aqueous systems and in hydrophobic mediums (e.g. plastic).

RESEARCH NEEDS

A systematic experimental investigation should be undertaken to measure the energy requirements to dewater nanocellulose suspensions, since the thermodynamics of water retention are likely non-linear with respect to the solids content. Such experiments would also benefit from a corresponding theoretical component to further elucidate molecular level origins of water retention and how they are impacted by salt and surfactant additives, temperature and pressure.

A comprehensive imaging-based investigation of nanocellulose redispersion is absent from the literature and would be extremely helpful to evaluate the efficacy of dewatering and redispersion methods.

SWOT analyses (Strengths, Weaknesses, Opportunities, and Threats) of dewatering and drying methods on a case by case basis for different applications would be beneficial. Given the wide array of potential applications for NC, the SWOT results will also vary greatly.

A Review of Nanocellulose Compatibilization for Polymer/Resin Composites35

Challenges

The review surveyed the Cellulosic Nanomaterial (CN) literature to seek out and identify approaches that successfully incorporate hydrophilic CN into hydrophobic polymer/resin matrixes via industrially viable methods for significant performance enhancements. With industry relevancy in mind, the review excluded compatibilization approaches that utilize complex or time consuming steps, solvent casting, toxic or difficult to work with solvents, high gravitational/rpm centrifugation, etc. as they are deemed not industrially viable. Also excluded were those approaches that resulted in insignificant improvements in mechanical performance.

An important background clarification is that CN extracted with sulfuric, phosphoric acid, or TEMPO (2,2,6,6 tetramethylpiperidinyloxy) are hydrophilic and ionic. This circumstance makes their handling fundamentally different from extraction methods that yield purely hydroxylated surfaces such as with hydrochloric acid. The ionic character of the CN generates a self-dispersing character in water whereas a native cellulose surface is less stable for long periods of time. However, this dispersion stability advantage poses a challenge when seeking to convert ionic containing surfaces to compatibility with hydrophobic polymers or resins. Thus,


the success or failure of a composite approach is dictated by how it addresses this and other issues. With this in mind, CN polymer composites are reviewed in three categories related to the CN starting material: 1) waterborne, 2) freeze dried, and 3) alternative. These categories refer to the process utilized in handling and preparing the CN for incorporation into polymers or resins. Waterborne stipulates that the CN is dispersed or conveyed in water and incorporated into resins etc. in a similar state. Freeze dried indicates that water was removed from CN via generally rapid freezing followed by sublimation of the water under reduced pressure yielding a powder that is utilized in further steps towards the composite. Freeze drying is highly time consuming. It is included in this review as the potential exists for other methods to fill its place, allowing the remainder of the procedure to be harnessed. The alternative category encompasses approaches that are neither of the former and generally differ from normative approaches.

Current State-of-Knowledge Summary

Waterborne Systems

As most CN extraction methods handle the cellulosic starting material in water and the CN product output in the aqueous state, using this directly in waterborne polymer systems without further modification is by default an easy path towards industrialization.

Strength improvements for WB CN systems have been reported for a variety of water-based latex and emulsion system including styrene/butyl acrylate co-polymers36, Acrylic37, natural rubber38, PE39 and epoxy40.

Freeze drying approaches

In efforts to move towards more hydrophobic polymer composites, researchers have endeavored to separate the CN from their aqueous medium and transform or compatibilize their hydrophilic surfaces. Freeze drying approaches are an effective laboratory-scale means of water

removal allowing further surface treatment of CN for improved incorporation into hydrophobic polymers. This methodology facilitates the investigation into how well CN perform as reinforcing phases in such materials. Strength improvements for a variety of freeze-dried nanocellulose polymer composites have been reported including polypropylene4142, low density polyethylene43, and poly-lactic acid444546. The methods employed to modify and disperse FD CN are quite varied

Alternative approaches

There is a great diversity in approaches that achieve CN surface functionalization or hydrophobic polymer incorporation without freeze drying or solvents that are toxic or difficult to remove. The approaches include one pot surface modification of CN aqueous dispersions to the hydrophobic state47, industrial spray drying4849, composite fabrication processes that utilize a slurry of CN in water or ethanol with a plasticizer added in some situations to improve compatibility50, and simple oven drying51.

KNOWLEDGE GAPS

Remaining challenges that must be overcome to advance both the manufacture and use of cellulosic nanomaterials in polymer/resin composites include:

Silane surface modification of cellulose is not as facile as with inorganic reinforcing materials. The ideal conditions for such chemistry to take place are aqueous hydrogen bonding of silanol oligomers to the surface of CN followed by heating over 100°C to cause condensation to a covalent bond. It seems unlikely that this second step would be efficient while the CN is in the aqueous state. Washing of the CN during water removal reportedly removes much of the hydrogen bonded silanol. Thus, alternative methods need to be developed indicating that the full potential of


silane modification of CN may not yet have been harnessed.

Concentrating of CN without agglomeration via industrially viable means is a challenge that once overcome could greatly facilitate their use in waterborne applications

A rapid drying process that produces easily redispersible CN is a challenge that once solved could greatly benefit nearly all CN endeavors.

Industrially scalable surface modifications on CN that produce a surface that is reactive with the matrix is a gap that could produce optimally performing polymer – CN composites. Maleic anhydride modified polymers is currently the most common way of achieving this.

What are the parameters and methods of achieving optimal spacing of CN within polymers for maximum performance enhancement?

What are the killer applications for CN that will allow it to break into the predominately petrochemical-based high performance composite markets?

RESEARCH NEEDS

No comparisons with industrial reinforcing phases were included in the reviewed literature. This may act as a significant barrier to industrial interest. Perhaps a benchmarking study should be undertaken to create industrially relevant polymer composite products with CN via methods discussed in this review or other suitable methods and compare them against similarly fabricated composites with currently used reinforcing phases.

Due to the diversity in CN extraction processes and sources it is vital that publications provide clear images of the CN in its final extracted and purified state prior to other

treatments. The CN should be diluted such that when deposited on a substrate for imaging they are not stacked on top of each other or intertwined. This will allow for ease of identifying the type of CN and its dimensions. This same procedure should be undertaken again after all processes and treatments have taken place and before and after incorporation into the composite so changes in dimension are accounted for.

The state of dispersion of the CN in the polymer is a vital aspect of its ability to provide reinforcement. Clear images of the state of dispersion in the polymer need to be provided. The birefringent nature of CN makes cross polarized optical microscopy ideal for evaluating the state of dispersion in optically transparent composites. Dynamic mechanical analysis (DMA) storage modulus above Tg appears to provide an indication of the state or effectiveness of the dispersion.

Un-surface modified CN – polymer composites may have faster and higher moisture uptake. How does this impact product performance and what can be done to control or mitigate it?

Research should be carried out to determine how susceptible CN-polymer composites are to fungal attack. Additionally, the impact of surface modification including hydrophobization and imparted reactive sites should also be evaluated.

Solvents need to be identified for use with CN surface modification that are readily removed via industrially scalable processes.

Methods or additives that assist in the disruption of CN self-affinity during dewatering and drying need to be investigated. Knowledge in this area would greatly facilitate their


incorporation in waterborne polymer products such as coatings.

Sedimentation of CN during waterborne natural rubber drying was frequently reported. Investigations should be carried out to discern how widespread his issue is and what can be done to mitigate it.

Research should be carried out to develop or discover compatibilizers that don’t sacrifice stiffness.


Session III: Opportunities

For the next session, four breakout groups were formed to review an assigned list of KNOWLEDGE GAPS and define RESEARCH NEEDS to address them. Participants were allowed to select KNOWLDEGE GAPS of most interest to them from the list. The breakout groups were tasked with brainstorming RESEARCH NEEDS (specific issues and challenges). Then they were asked to consolidate and prioritize the RESEARCH NEEDS for impact and time to implement.

The initial list of KNOWLEDGE GAPS for each breakout group were derived from R&D KNOWLEDGE GAPS identified by the literature review authors and those identified by participants that should be discussed in Session III as they were able to identify them during the literature review presentations.


R&D KNOWLEDGE GAPS -- Drying & Dewatering

Breakout Group #1 Breakout Group #2

Drying of NC such that it is completely redispersible in water has been developed for certain specific applications of NC, but the successful examples seem to be costly. This cost could potentially be justified for a high-value product. Techno-economic analyses will be needed for each case. A general techno-economic (TE) model is needed that includes variable costs and product valuations, or a set of example TE studies for various promising applications.

We lack drying technologies and processes that are scalable, low-energy and cost-effective and that preserve NC properties following re-dispersion in aqueous systems or dispersion in hydrophobic mediums (e.g., plastic).

While some techniques to aid in dewatering were found in the literature, it is not clear at what threshold solids content the NC-water mass can be still be completely redispersed without the need for any special measures such as sonication, high-shear mixing, or the use of additives.

Are there any lower-cost redispersion methods for cellulose nanofibrils (CNF) that would be appropriate for commodity industries such as paper?

How to dry nanocellulose hydrogel so that it immediately re-swells in water?

When additives are used to enhance dewatering and drying and need to be removed; additive removal processes aren’t well developed.

What are the interactions between water and the surfaces of NC? We need to better understand the nature of association and bonding.

Integration of drying with membrane separations to pre-concentrate suspensions prior to drying (avoid centrifuge) that avoid fouling of membrane.

When additives are used to enhance dewatering and drying, we need to be able to control additive coverage and protrusion from surface.

How do end products/intended end uses alter available drying techniques, processes, or acceptable additives?

We need a better understanding of the structure of concentrated suspensions.

How strongly is water held on the different morphologies, such as crystalline or amorphous surfaces?

We need to understand the phase behavior in the system: NC/water as a function of size, temperature, additives….

We need methods to quantify redispersability.

Surfactant or additive recovery if necessary is very challenging, but possible. Some approaches include chromatographic ion-exchange and ionized surfactant de-adsorption.


R&D KNOWLEDGE GAPS -- Compatibilization


Why isn’t silane surface modification of cellulose as facile as with inorganic reinforcing materials? Methods of silane modification of CN are not well developed.

We lack industrially scalable surface modifications for CN that produce a surface that is reactive with the polymer/resin matrix in order to produce optimally performing polymer-CN composites.

What are the parameters and methods of achieving optimal spacing of CN within polymers for maximum performance enhancement? Is this more than simply achieving complete dispersion?

What are the killer applications for CN that will allow it to break into the predominantly petrochemical-based composites markets?

Methods of compatibilization of CN with other nanoparticles are needed.

How can we translate academic research into viable industry products?

We lack understanding of the impact of CN on long-term stability of polymer/resin composites.

In what ways can we bridge lab experiments to small- or large-scale production?

Fundamentally, why is dispersion so important for physical properties?

What are the main drivers responsible for mechanical reinforcement? Is surface chemistry, dimension, or dispersibility more important? What is the influence of environmental conditions?

Is compatibilization really what we are looking at for maximizing interfacial adhesion in polymers?

How do we observe NC inside of a polymer matrix?


Priority RESEARCH NEEDS

Participants in each breakout session then brainstormed pre-competitive RESEARCH NEEDS to address the KNOWLEDGE GAPS and ranked the RESEARCH NEEDS according to implementation time and anticipated impact of the research towards.

commercialization (e.g. a critical fundamental understanding that would advance the field).

The priority pre-competitive RESEARCH NEEDS identified by each breakout group ranked according to commercialization impact are provided in the tables below.


Priority RESEARCH NEEDS -- Drying & Dewatering


1. Quantify cost/energy expenditure of drying a well-defined NC standard compared across various drying methods; Techno-economic analysis at varying levels of solids content (10% vs 50% vs 95%)

1. Increase fundamental understanding of water/CN interactions, and stage at which hydrogen bond interactions start being a factor

2. Characterization of dewatering and drying across the range of NC materials (structure-processing-property relationship differences in varying NCs)

2. Develop understanding of how to interfere with hydrogen bond formation during drying processes

3.Establish phase diagrams (normalized by surface area) of the varying NC-water interactions

Types of water (bound versus frozen versus unbound)

Computational: bound-water conformation on NC crystal facets

Experimental: characterization (NMR, DSC, dielectric measurements, etc)

3. Common terminology to describe dispersion/redispersion and characterization across various applications

4. Time vs. expense to redisperse NC

Determine methods to quantify dispersion ; concentration required for optimal dispersion

Establish techniques, processes, and orders to render most efficient dispersion

4. Dehornification mechanisms and methods (can CN agglomerates be broken by various methods)?

5. Cost analysis and alternative dewatering and drying methods


Priority RESEARCH NEEDS -- Compatibilization


1. How to silane-functionalize CN in the absence of a water or solvent phase.

1. Industrially scalable surface modifications (SM) on CN that produce a surface that is reactive with the matrix.

2. Develop compatibilizing or functional surfaces on CN without silane as organic solvent.

2. What are the killer applications for CN that will allow it to break into the predominantly petrochemical-based composites markets?

3. How to understand the relationship between dispersion and performance and how this is affected by scale-up.

3. In what ways can we bridge lab experiments to small- or large-scale production?


Session IV & V: Researchers & Realizers

The event also showcased US capabilities in nanocellulose R&D, production and applications development. Appendix D provides a catalogue of active US-based nanocellulose community members along with their area of focus, expertise and unique assets in the field.

More than two dozen suppliers and users gave rapid-fire presentations of their capabilities and a number provided posters for review during an interactive networking luncheon. See Appendix E for a list of presentation titles and speakers.

Session VI: Making it Happen - R&D Projects to Address RESEARCH NEEDS

The breakout groups developed the preliminary research plans provided below to address the high-priority RESEARCH NEEDS. The intention of the project plans was to inspire additional thinking about solutions and motivate stakeholders to form collaborative teams to take action to address these RESEARCH NEEDS.

For sake of clarity the research plans, created by each team individually, have been consolidated to eliminate overlap.

Readers of this report are encouraged to contact APPTI if they have interest in accelerating or participating in these or similar R&D projects?


Dewatering & Drying Project Plan – Techno-Economic Analysis

KNOWLEDGE GAP Addressed: RESEARCH NEED Addressed:

More technologies and processes are needed to achieve scalable, low-energy, cost-effective preservation of NC fibril properties during drying for re-dispersion in aqueous systems and in hydrophobic mediums (e.g., plastic). Techno-economic (TE) analysis is needed for both dewatering and drying well-defined NC standard materials.

Quantify cost/energy of dewatering and drying prior well defined NC materials across different processes; coupled to comparison of varying processes, techno-economic analysis at varying levels of solid content (10% vs 50% vs 95%)

Project Objectives:

Provide an understanding of cost and performance of various drying and redispersing approaches for different applications.

Define application needs, constraints and process methodologies to provide the requirements for the material. Characterize each in terms of cost, scalability, dispersibility, industrial readiness, regulatory constraints, etc.

Project Outcomes & Performance Metrics:

Proposed R&D Effort / Technical Scope Summary

Cost of dewatering/drying for a given method to produce a quality product sufficient for a given end use application with current technology

Identification and evaluation of alternative technologies

General TE model for a given nanocellulose and process, listing the drying time, drying rate, cost and energy expenditure

Current State of Technology & Knowledge: Contacts for Follow-up by APPTI:

Multiple individual publications but nothing combined

Limited knowledge base available in terms of science as well as techno/economic analysis

Professor Ronalds Gonzalez – Supply chain and conversion economics (NC State)

Soydan Ozcan - ORNL

Project Plan:

Understanding cost/energy of today’s technologies

Definite alternative technologies that are available, outside of current NC drying techniques

Feasibility test/study

Identifying key needs for disruptive drying technologies


Dewatering & Drying Project Plan – Structure-Process-Property Relationships


How do the different forms of NC affect the way it dewaters, dries and aggregates?

Fundamental characterization of NC (structure-process-property relationship of varying NCs)

Phase diagram (as a function of surface area) of the varying NC-water interaction. Understanding bound water and conformation

Identify /stipulate specific NC structure and characterize behavior during the dewatering and drying process (difference for fibrils from crystals and difference in crystals/polymorphs)

Project Objectives:

Ensuring target performance of a particular form of nanocellulose after drying based on the specific application.

Project Outcomes & Performance Metrics: Proposed R&D Effort / Technical Scope Summary

An understanding of the relevant parameters that drive dewatering and drying and how drying and dewatering affect those relevant parameters.

Identifying the relevant parameters that can be measured that characterize and predict dewatering & drying performance

Understanding how dewatering & drying affects those fundamental parameters


Academic and government groups are beginning to establish reference NC materials and characterizing said materials

There are emerging activities in industry identifying relevant performance metrics that could mitigate scale-up issues.

There have been techniques that have been defined, but which of these techniques apply for each end use application have not been correlated.

Linda Johnston (NRC Canada)

Foster et al. Chem. Soc. Rev. VA Tech 47(8) (2018): Current characterization methods for cellulose nanomaterials

Tappinano.org/whats-up/standards-summary

Project Plan:

Review initial work on how water is bound to cellulose and couple this with computational studies.

There are currently basic products in the market that are readily available - attain these and perform fundamental characterization (size, zeta, viscosity)

Perform identical dewatering and drying method among the various forms of NC o Important to highlight what dewatering and drying method is being used and why

Once dewatering and drying has completed – determine if there is change in relevant properties

Understanding bound water and conformation

Types of water (bound versus frozen versus unbound)

Research need: computational of water bound and conformation on varying NC or experimental characterization (NMR, DSC, Dielectric measurements)


Dewatering & Drying Project Plan – Water/CN Interactions


We lack drying technologies and processes that are scalable, low-energy and cost-effective and that preserve NC properties following re-dispersion in aqueous systems or dispersion in hydrophobic mediums (e.g., plastic).

Increase fundamental understanding of water/CN interactions, and at what stage do hydrogen bond interactions start being a factor? Develop understanding of how to interfere with hydrogen bond formation during drying processes

Project Objectives:

- Determine if it is possible to detect single hydrogen (H) bonds. Measure H-bond formation and breakage between CNFs/CNCs and with other molecules in the surrounding environment.

- Determine where H bonds form first – along which face of the CN molecule and particle structure. Expecting there are multiple types of H bonds; develop understanding of unique characteristics of the nature of H bonds in cellulose.

o What are the appropriate experimental approaches to test that? o What are the appropriate modeling approaches? o Need to address environmental variables that affect H bonding in CN materials+



Ability to visualize hydrogen bonding process, in 3D – e.g., 3D tomography along lines of NIST’s work on visualizing carbon nanomaterials.

Modeling to provide visualization of how the bonding process takes place.

Ability to experimentally detect H bond formation, using experimental tools such as AFM, chemical methods.

Microscopic definition of hornification (irreversible bonding) during the drying process, and understanding of relation of that to hydrogen bonding kinetics between crystals.

Single particle analysis and then multiple particle kinetics analysis.

Thorough literature review – a lot of relevant work has already been done. What are the appropriate tools/instruments/models for measuring this?

Tweak the models for CNC and CNF- unique issues

Integrate spectroscopic techniques for measuring H bonding – is there a way to distinguish between different OH groups on different carbons. Consider NMR. Sum frequency generation spectroscopy? (only detects water at an interface, a couple of layers thick)

Current State of Technology & Knowledge: Contacts for Follow-up:

There is some work that has been done on molecular dynamics modeling of hydrogen bonding. Canadian group?

First paper on single H bond formation measurement, by high-res AFM, was published in 2017. In Basel, CZ.

Some existing papers on modeling of individual CNC crystals in water. (KTH and NREL? – or ORNL – presented at the recent ACS meeting.)

Kondo et al., 2017, Characterization of individual hydrogen bonds in regenerated cellulose, ACS Omega.

Robert Moon, FS Carson Meredith, GA Tech


Project Plan:

- Provide a summary description of the current state of the art associated with the research need.

- Take dewatering to incremental stages; in situ monitoring of the drying process - Do that with different types of drying [linked to given or known industrial scale methods] - Characterize with optics, chemistry, wide angle and small angle x-ray diffraction to

determine structure, crystal configuration, and spacing. - Adjust environmental parameters/chemistry and repeat – see what happens, hope that

affects the bonding process/rate. If you add impurity, different chemistry, that may affect the bonding process.

- See if any of those tweak either accelerate or retard H bond formation. - Timeframe: This is a long-term fundamental research project. - Likely interested agencies: DOE and NSF might have appropriate programs and

resources (DOE facilities for M&S, modeling and experiments in parallel). - Level of effort: on the order of $1 million per year, a team effort. Primarily an academic

effort.


Dewatering & Drying Project Plan -- Redispersion


We lack drying technologies and processes that are scalable, low-energy and cost-effective and that preserve NC properties following re-dispersion in aqueous systems or dispersion in hydrophobic mediums (e.g., plastic). What are the critical threshold of solid content in drying process where redispersion additive/measures are required (monolayer of water versus double layer etc.?)

Common terminology to describe dispersion/redispersion and characterization for various applications

Time; how long does it take to redisperse the given NC vs expense ; “redispersion thermo-kinetics”

Project Objectives:

Being able to address situation where customer asks: “How do I use this?” i.e. understanding the implementation of NC from fabrication to end product.

Having 100% recovery of dispersion of NC product after dewatering drying or a recovery based on fit-for-use for the end application.

A standardized definition and approach for describing dispersion. How do you define solution? Are there particles? Is there agglomeration? If you dewater it and then dry it, do you have the same material? How do the requirements differ in polymer systems, in aqueous systems?

Standard Operating Procedures (SOPs) for redispersing and characterizing the dispersion



A common definition of dispersion and industry standard specifications for different materials and applications

Understanding the relationship between redispersion process and critical variables and the overall extent of dispersion

Parallel: understanding fundamental mechanisms that describe redispersion

Identify specific threshold of dispersion necessary for any given end product Develop stronger understanding of the kinetics and the amount of energy required for dispersion using varying techniques


Many different specifications and methods for characterizing are used – not comparable.

Joe Miller offered the following example of what another industry has done: Link to NIST Report Soydan Ozcan, Robert Moon, Joe Miller, Michael Reznikov, Anna Carlmark

Project Plan:

Common Terminology/Measurement

Define customer needs

Develop specifications for different materials and applications Redispersion time

Quantify the consistency of redispersion; what concentration are required for optimal dispersion (higher concentration often more easy to redisperse)

Determine what techniques, processes, and orders will render most efficient dispersion

https://tsapps.nist.gov/notifyus/docs/wto_country/PHL/full_text/pdf/PHL100(english).pdf


Plastics Compatibilization Project Plan – Functionalizing with Silane


Why isn’t silane surface modification of cellulose as facile as with inorganic reinforcing materials?

Develop approach to silane functionalize CN in the absence of a water or solvent phase

Project Objectives:

Silane functionalize CN with a high degree of surface functionalization and specificity in the absence of water or solvent phase leading toward industrial application.



Silane functionalization works with improvements in performance, strength, durability of the matrix

Expected to work for specialty materials and intermediate volume plastics but not commodity plastics, e.g. not HDPE

A viable and efficient process in terms of material usage and yield

An economically viable process with a favorable cost/benefit ratio

Materials – CNC, CNF, CMF and surface derivatives; in never-dried state

Products – plastics

In-situ modification (during production of CNs) or silanization integrated into CN production

Learn to use silane chemistry that is compatible with cellulose – some of these are polymers themselves

Current State of Technology & Knowledge:

Contacts for Follow-up by APPTI:

Silane chemistry is known and preferred industrially. The question is the ability to use it with CNs to improve compatibility with plastics.

Polymer processing companies

Silane users – given that it is being used industrially

Project Plan:

Select product targets and materials of interest

Evaluate alternate approaches based on those being used in other materials o Are any aqueous phase reactions available? o Can vapor phase reactions be applied in steam explosion aerogel? Is anything that is

being done with CMC relevant? Issue – can we get a source of CNs that doesn’t result in encumbered IP material with a

limited use?


Plastics Compatibilization Project Plan – Functionalizing without Silane


We lack industrially scalable surface modifications for CN that produce a surface that is reactive with the polymer/resin matrix that will produce optimally performing polymer-CN composites.

Develop compatibilizing functional surfaces on CN w/o silane or organic solvents

Project Objectives:

Determine the attributes of dispersion that improve performance.

Determine how to functionalize the surface for each matrix of interest and the best agent and conditions for matrix.

Project Outcomes & Performance Metrics: Proposed R&D Effort / Technical Scope Summary

Demonstrates improvements in performance, strength, durability of the matrix

Expected to work for specialty materials and intermediate volume plastics and also for commodity plastics,

A viable and efficient process in terms of material usage and yield

An economically viable process with a favorable cost/benefit ratio

Demonstrates good rheological behavior.

Determine materials to be included. o Polyolefins? o Polyesters including biobased?

Determine performance improvements required to be of interest?

Packaging could be a good target – renewable, biodegradable, compostable, etc.


Can available chemistry be brought to scale? Some have serious drawbacks (hazardous chemistries, high energy, high cost)

Compatibilizers can reduce performance

Functionalization not reactive with matrices

Current systems generally limited to maleic anhydride

Chemistry not sufficiently stable or can mitigate

One pot is not ideal for resins

Polymer processing companies

Project Plan:

Adjust chemistry to matrix. Select based on solubility and modeling. Chemistries currently being evaluated – maleic anhydride, enzymes, emulsion

Address issues with negative impact on recycling – or claim that it must be compostable

Can we make these with high levels of CNs – 30-40%? (There might be opportunities for high level – not just 1-2%).


Plastics Compatibilization Project Plan – Killer Applications


What are the killer applications for CN that will allow it to break into the predominantly petrochemical-based composites markets?

Determine where CN can provide an economically viable benefit including materials for reducing weight in transportation

Project Objectives:

Identify target applications based on benefits, cost and compatibility with existing systems



Demonstration of economic benefits in terms of weight reduction and fuel savings

Demonstrate compatibility with current assembly/repair processes (no additional steps in manufacturing process)

Higher performance at same or lower system cost

Improve life cycle assessment of part or vehicle through lower cost, extended functional life, lower end of life cost

Collaborate with an industry partner/mentor

Identify parts and materials of interest - discovery / development / characterization

Conduct part specific performance testing versus standards and specs

Develop scale up approach

Current State of Technology & Knowledge:

Contacts for Follow-up by APPTI:

Material usage is mostly thermoplastics in autos with more thermosets in aviation

There is very little experience with cellulosics

There is market pull for more sustainable solutions

Tier 1, 2, and maybe 3 suppliers are new technology gate keepers

Eric Mintz

Roland Gong

Meisha Shoffner

Paul Latten

Project Plan:

ID target parts in transportation segments (structural vs non-structural; likely interior)

Benchmark part & system cost

Define target weight reduction

Determine current and future life cycle.

Understand and address EH+S hurdles (material handling, assembly, use)

Demonstrate technology works


Path Forward

This workshop builds on past efforts by USDA Forest Service, the National Nanotechnology Initiative, and APPTI to explore the market potential of cellulose nanomaterials applications and enable commercialization through R&D advancement.

The specific focus of the workshop was to determine critical KNOWLEDGE GAPS and RESEARCH NEEDS for the priority RESEARCH AREAS relating to nanocellulose drying and dewatering and interfacial compatibilization with plastic composites, which, if overcome, would have the greatest impact on accelerating widespread implementation and commercialization of nanocellulose materials and applications.

A central goal of this workshop was to define the current state-of-knowledge in the priority RESEARCH AREAS and deconstruct the identified KNOWLEDGE GAPS into RESEARCH NEEDS, or specific technical issues and challenges that, if solved, would have the greatest impact on closing the KNOWLEDGE GAPS and lead to breakthroughs or new technology solutions to advance nanocellulose commercialization. The workshop enabled input from a wide range of stakeholders and facilitated a collaborative dialogue across government, academia, and industry.

R&D project plans were developed by workshop participants to address the priority RESEARCH NEEDS that define the project objectives, outcomes, performance metrics, current state of technology and knowledge, and activities to be conducted over the life of the project to execute the project scope and meet the project objectives. The project plan are intended to inspire formation of collaborative teams to take action to address the priority RESEARCH NEEDS.

The R&D project plans will be used by APPTI’s Cellulosic Nanomaterials team and supporting partners for next-stage planning of projects that support development of pre-competitive technology platforms that enable new revenue streams from forest-based biomass. Readers of this report are encouraged to contact APPTI if they have interest in accelerating or participating in these, or similar? R&D projects.

As evidenced by over 65 workshop participants representing a broad range of US-based stakeholders within the nanocellulose field, there is a diverse community of engaged players with exceptional expertise and capabilities within our nation. APPTI encourages the formation of a more formal network of US-based stakeholders to elevate nanocellulose research and commercialization efforts by connecting stakeholders and fostering new collaborations.


Appendix A - Workshop Organizing Committee

Alex Beam Domtar Kathleen Bennett Alliance for Pulp & Paper Technology Innovation Jim Dewitt SAPPI Lisa Friedersdorf National Nanotechnology Coordinating Office Geoff Holdridge** National Nanotechnology Coordinating Office Mike Kiley National Nanotechnology Coordinating Office Brad Langford** Domtar Nathalie Lavoine North Carolina State University Lester Li SAPPI Clare Mahoney** National Nanotechnology Coordinating Office Kim Nelson* GranBio Technologies World Nieh USDA Forest Service Soydan Ozcan** Oakridge National Laboratory Greg Schuneman** USDA Forest Service Forest Products Laboratory Meisha Shofner** Georgia Institute of Technology Scott Sinquefield Georgia Institute of Technology David Turpin** Alliance for Pulp & Paper Technology Innovation Steven Winter International Paper Colleen Walker* University of Maine *Workshop Co-Chairs

** Session Chairs


Appendix B - Workshop Participants

Name Company

Paul Albee P3N Technology Inc

Dwight Anderson International Paper

Dilpreet Bajwa North Dakota State University

Cosmas Bayuardri GranBio

Greg Becht Croda Inc

Kathleen Bennett KMB Consulting

Richard Berrry CelluForce

Hongda Chen USDA NIFA

David Cowles GLV USA Inc.

Yulin Deng Georgia Institute of Technology

Michael Easson USDA, ARS, SRRC

Sean Eicher GEA Westfalia Separator Group GmbH

Douglas Fox American University

Lisa Friedersdorf National Nanotechnology Coordination Office

Alex Friend USDA Forest Service

Douglas Gardner University of Maine

Ashok Ghosh Westrock

Micheal Goergen US Endowment for Forestry and Communities

Roland Gong University of Wisconsin - Stevens Point

Erkki Hellén VTT

Geoff Holdridge National Nanotechnology Coordination Office

You-Lo Hsieh University of California, Davis

Jim Hubbard US Department of Agriculture

Maria Celeste Inglesias

Auburn University

Alexander Kraus GEA Westfalia Separator Group GmbH

Bernard Lager Insight Bioscience Innovations

Panu Lahtinen VTT

Bradley Langford Domtar

Paul Latten Southeast Nonwovens, Inc.

Nathalie Lavoine NCSU Forest Department

Kai Li Oak Ridge National Laboratory

Lester Li SAPPI

Clare Mahoney National Nanotechnology Coordination Office

Anna Carlmark Malkoch

RISE Research Institutes of Sweden

Jonathan Markley Evergreen Packaging

Carson Meredith Georgia Institute of Technology

Name Company

Jack Miller Biobased Markets

Joseph Miller Inqubator Consulting

Sergiy Minko University of Georgia

Eric Mintz Clark Atlanta University

Robert Moon USFS-Forest Products Laboratory

World Neih USDA Forest Service

Kim Nelson GranBio

Soydan Ozcan Oak Ridge National Laboratory

Shaobo Pan GranBio

Sunkyu Park North Carolina State University

Dom Porcincula California Polytechnic State University, San Luis Obispo

Arthur Ragauskas University of Tennessee

Michael Reznikov Physical Optics Corporation

Carlos Rodriguez Franco

USDA Forest Service

Veikko Sajaniemi Poyry Management Consulting

Greg Schueneman USFS-Forest Products Laboratory

Mark Shmorhun Department of Energy

Meisha Shofner Georgia Institute of Technology

Stephen Sikirica Department of Energy

Scott Sinquefield RBI at Georgia Institute of Technology

Stacey Standridge National Nanotechnology Coordination Office

David Turpin APPTI

Yocheved Ungar Columbia University

Santosh Vijapur Faraday Technology, Inc.

Colleen Walker University of Maine

Yu Wang Oak Ridge National Laboratory

Siqun Wang University of Tennessee

Steven Winter International Paper

Shanju Zhang Cal Poly-San Luis Obispo

Junyong Zhu USFS-Forest Products Laboratory


Appendix C - Workshop Agenda

Day One: Assessment, Challenges and Priorities

TIME TOPIC

8:00-8:15 Welcome & Introduction Purpose of workshop; charge to the group David Turpin, Executive Director - APPTI

8:15-9:45

Session I: Emergence of the Nanocellulose in the Bioeconomy Welcome and Overview – Lisa Friedersdorf, National Nanotechnology Coordination Office

US Forest Service Interest In Cellulose Nanomaterials – Alexander Friend

Importance of Cellulosic Nanomaterials to the Bioeconomy and to Forests and Rural Communities – Jim Hubbard, Under Secretary for Natural Resources and Environment, US Department of Agriculture

Progress in Global Commercialization of Nanocellulose – Jack Miller, Market-Intell

End-User Commercial Needs – Colleen Walker, University of Maine/Kim Nelson, GranBio

Innovation Is Challenging: Crossing the Valley of Death – Michael Goergen, Vice President – Innovation and Director, P3Nano, US Endowment for Forestry and Communities

9:45-10:00 Break

10:00-12:30

Session II: Challenges Drying and Dispersion Literature Review Scott Sinquefield, Renewable Bioproducts Institute – Georgia Tech

Compatibilization Literature Review Greg Schuenemann, US Forest Service – Forest Products Laboratory

12:30-1:30 Lunch and Networking

1:30-4:30 Session III: Opportunities Participants review list of knowledge gaps and define research needs to address

1:30-3:30 Participants select gap area of most interest from a list to be provided. Breakout groups brainstorm approaches, sort for promising areas, consolidate, prioritize for impact and time to implement. A participant agrees to report for the group.

3:30-4:00 Break All participants review rankings and priorities from all breakout groups; note reactions to others’ results

4:00-4:30 Regroup and discuss (All workshop participants) Volunteer reporters from each group report results; participants share their reactions and suggestions

4:30-5:00 Putting it Together Summary of Day One; charge for Day Two

5:30-7:00 Offsite Reception The Brighton


Day Two: Resources, Opportunities and Research Plan

TIME TOPIC

8:00-8:05 Introduction Recap of Day One results; plan and outcomes for Day Two

8:05-9:45

Session IV: Researchers & Realizers Session Introduction Flash reports: Representatives of US capabilities give five-minute reports, max three slides, sharing their areas of expertise, progress, and capabilities. Posters are displayed at lunch for audience members to review.

9:44-10:00 Break

10:00 – 11:30 Session IV, Continued

11:30-1:30 Session V: Lunch & Poster Session Participants enjoy lunch while reviewing posters of the morning’s presentations; engage in further networking

1:30-1:45 Introduction to Work Session Recap of Day One results and morning discussion; instructions for the afternoon

1:45-4:00

Session VI: Making It Happen Participants return to their breakout groups and begin to identify plans for executing research on the high-priority approaches, using a template to be provided: identify expertise, experts, and capabilities needed; outline research targets and milestones; lay out other next steps that would enable preparation of an APPTI Request for Proposal

4:00-4:30 Path Forward Summary; next steps; group discussion about accomplishment of workshop deliverables


Appendix D - US Capabilities and Expertise

Name Title Organization Nanocellulose focus/expertise Nanocellulose R&D Assets Email

Alexander Kraus Product Sales Manager Chemicals

GEA / GEA Westfalia Separator Group GmbH

Equipment for separation and dewatering of nanocellulose, several equipment provided for liquid – solids separation

product trials carried out [email protected]

Art J. Ragauskas Professor/Governor’s Chair in Biorefining

University of Tennessee

Structurally engineered nanocellulose composites with environmentally responsive features

State-of-art laboratory facilities for production and characterization of CNC/CNF from assorted feedstock and incorporation into printed composites

[email protected]

Bernard Lager II Director of Technology

Insight Bioscience Innovations

Focus is on dewatering and drying of Nanocellulose and composites.

We have laboratory drying including a pilot scale multi-phase dryer capable of drying lab samples up to production volumes. We also have several large scale dryers capable of drying commercial volumes.

[email protected]

Brian Via Director Auburn, Forest Products Development Center

Wood Composites [email protected]

Carson Meredith Professor Georgia Tech modification, barrier materials, hybrids with other biomass-derived materials

Pilot-scale homogenization, coating facilities, high-throughput property screening

[email protected]

Christie Sayes, PhD

Associate Professor

Baylor University Physicochemical characterization, interactions/reactions with organisms (rodent, cell cultures, zebrafish), formulation testing, surface functionalization & characterization

Microscopy (electron, light, tunneling, force), spectroscopy (light scattering, UV-Vis-IR, energy dispersive, fluorescence), mass spectrometry, diffraction (electron, X-ray); zebrafish colony, sprague Cawley rat colony, human mammalian cell colonies (respiratory, gastrointestinal, neurological, liver, kidney, dermal)

[email protected]

mailto:[email protected]





http://nsmlab.com/







Colleen Walker Director, Process Development Center

University of Maine

production, applications development and commercialization

1 tpd pilot plant with expansion in 2020 for continuous production and larger scale, lab and “pilot” scale supermasscolloider, pilot paper machine, pilot coater, a wide range of analytical and testing capabilities

[email protected]

David Cowles Global Business Manager, Nanotechnologies

Valmet, formerly GL&V

MFC production using refiners, both conical and disk. MFC application which includes internal addition and surface application.

Alliance with University of Maine that includes various production methods from bench top to commercial in addition to the pilot machine and coater. In addition, nanocellulose research and application research is being done at the university included within various departments. Within Valmet we have various MFC production options, 2 high speed pilot machines that can be configured various ways, 1 high speed tissue machine that can be configured multiple ways, and additional options for pilot coater research. Valmet also offer skid refiners for rental and MFC applicators for commercial trials.

[email protected]

David Turpin Executive Director

Alliance for Pulp & Paper Technology Innovation (APPTI)

Identification of common pre-competitive technology challenges, that if solved would enable proprietary commercial development of cellulosic nanomaterials. Prioritizing and communicating research needs. Identifying sources of funding to address the challenges.

Alliance of companies committed to commercialization of cellulosic nanomaterials.

[email protected]







Dilpreet Bajwa, Ph.D.

Professor Montana State University

Nanocellulose functionalization, Processing, Applications in Fire Retardants, Soft Materials (hydrogels), and Polymer Composites

Material Processing (Extruder, Injection molder, Compression Molder, Homogenizer, Ultrasonicator), Characterization (DMA, DSC, TGA, FTIR, NMR, TEM/SEM, Goniometer, and NMR, Instron, Q-Sun weather-o-meter) and general laboratory equipment.

[email protected]

Douglas Gardner Professor University of Maine

drying, surface modification, cellulose nanocomposites, electrospinning, 3D printing, packaging applications

Nanocomposites Lab, pilot scale spray dryer, large scale 3D printer, extrusion capabilities, analytical lab: thermal analysis, rheometry, microscopy, IGC, AFM, laser diffraction, mechanical testing, durability testing

[email protected]

Douglas M. Fox Professor of Chemistry

American University

Nanocellulose labeling for tracking migration or distribution and surface modification to improve interfacial interactions, reduce water uptake, and increase thermal stability

Electron, fluorescent, and Raman microscopy, thermal analysis and calorimetry (TGA, DSC, DMA), Spectrometers, XRD, BET, and access to NIST (Gaithersburg, MD) instrumentation

[email protected]








E. Jennings Taylor, PhD

Founder & CTO Faraday Technology, Inc.

Low cost electrochemical dewatering of nanocellulosic materials.

Extensive intellectual property portfolio (patents, trademarks, service marks and know-how) covering various embodiments of pulse/pulse reverse electrolytic processes including a patent pending directed towards a method and apparatus for dewatering of cellulosic nanomaterials. Capabilities and facilities include process development from bench-scale to pre-production prototypes. Faraday’s commercialization strategy for the FARADAYIC® Electro-DeWatering process and FARADAYIC® Electro-DeWatering apparatus is to license and/or selling the relevant patents.

[email protected]

Eldho Abraham PhD

Research Associate

University of Colorado Boulder, USA

Nanocellulose production from wood-pulp, natural fibers and bacterial cellulose from agricultural and food waste resources

Working with Advanced Research Projects Agency-Energy (ARPA-E) for flexible 99% transparent polysiloxane-nanocellulose aerogel for window energy saving window application, greenhouse energy saving application, thermal insulator materials application

[email protected]

Eric A. Mintz, Ph.D.

Professor of Chemistry

Clark Atlanta University

Preparation and Characterization polymer matrix composite incorporating nanocellulose.

Lab scale processing; melt mixer, single and twin screw extruders, film blowing tower, hot press. Characterization, melt rheometer, DSC, TGA, TMA, DMA, tensile testing, optical microscopy, IR, NMR, XRD (with hot/cold stage).

[email protected]






Greg Schueneman

Supervisory Materials Research Engineer

: USDA USFS Forest Products Lab

Surface modification for composites

My brain (such as it is) [email protected]

Gregory Becht, Ph. D.

Lead Application Scientist

Croda Inc. Nanocellulose application development in printing and electronics areas

Mostly physical testing (rheology, contact angle, surface tension), also partnering with industrial sector to drive nanocellulose into the field

[email protected]

Halil Tekinalp R&D Staff Oak Ridge National Lab

Nanocellulose production, drying, composites applications, additive manufacturing applications

In conjunction with UMaine, nanocellulose production/fibrillation, surface treatment, spray drying, compounding, composite and additive manufacturing application capabilities

[email protected]

Howard Fairbrother, PhD

Professor (Chemistry)

Johns Hopkins University

Functionalization of Nanocellulose, Biodegradation and Mechanical Properties of Nanocellulose/Polymer Composites

Chemical apparatus for nanocellulose functionalization, characterization (FTIR, XPS, DSC/TGA, SEM)

[email protected]

J.Y. Zhu Scientific Team Leader

USDA Forest Products Lab.

Sustainable Production of lignocellulosic Nanomaterials/Lignin nanoparticles (LNPs)

Several US patents on sustainable production of cellulose nanomaterials, including solid maleic acid hydrolysis process for producing carboxylated nanomaterials from commercial pulp fibers, as well as from wood/raw biomass directly. Pilot scale reactors, homogenizers, disk refiners for treating fibers, producing cellulose nanomaterials. Characterization (Dynamic light scattering/zeta-potential, DSC/TGA, NMR, SEM, AFM, AFM-Raman, Raman), physical property tests (Instron, DMA).

[email protected]











Jack Miller Principal Consultant

Biobased Markets

Nanocellulose markets, market analysis, market research, marketing, and business development

Extensive network of nanocellulose experts including producers, universities and research centers, plus end users and potential customers for nanocellulose producers

[email protected]

Jeff Gilman, PhD Project Leader NIST functionalization, analysis, self-assembly

Nanocellulose R&D Assets: extensive measurement science facilities

[email protected]

Jeffrey P. Youngblood

Professor Purdue University

Nanocellulose composites fabrication and testing, Nanocellulose in cement, Nanocellulose in packaging, Nanocellulose fundamental properties.

Common thermal (DSC, TGA), mechanical (Instron, DMA, Rheometers), chemical (NMR, Raman) and structural (Zetasizer, X-ray, SAXS, SEM,TEM, AFM) characterization and processing (high shear mixer, conical twin screw compounder, single screw extruder) equipment

[email protected]

Jo Anne Shatkin President Vireo Advisors, LLC

novel product safety requirements, regulatory requirements and authorizations, international consortia development and coordination, nano-specific safety methods development, application specific safety data and packages, surveillance and global market developments, proactive work to promote more efficient/safer commercialization, bioeconomy and sustainability analysis, life cycle risk analysis, toxicology, technical communications

databases of safety data, safety data sheet templates, expertise, networks/established collaborations - academic/government/industry internationally

[email protected]











Kim Nelson CTO Nanocellulose

GranBio, formerly American Process Inc.

Nanocellulose production, application development and commercialization

GranBio's Thomaston Biorefinery produces up to 1/2 ton per day BioPlus® of five different nanocellulose products with the patented BioPlus with AVAP® and BioPlus with GreenBox® processes.

[email protected]

Maria Soledad Peresin

Assistant Professor

Auburn University

cellulose nanofibrils production and characterization, surface interactions, surface chemistry, rheology; applications: water remediation, sensing, adhesives, nanocomposites, electrospinning, hydro/aerogels

facilities for CNF production: Masuko Supermasscolloider. Characterization techniques: zeta potential, charge density, thermal properties (TGA, DSC), chemical properties (FTIR), surface free energy (CAM), morphology (AFM, SEM). Surface interactions: Quartz Cristal Microbalance (QCM-D).

[email protected]

Mi Li, PhD Assistant Professor

University of Tennessee Institute of Agriculture

Nanocellulose production, chemical modification, and functionalization

CNF/CNF production (disk homogenizer), synthesis glove box, characterization (IR, GPC, DSC/TGA, X-ray, NMR, SEM/TEM, polarized microscope, rheometer, Instron, DMA)

[email protected]

Michael E. Himmel

Senior Fellow National Renewable Energy Laboratory

Nanocellulose preparation/separation/characterization with general expertise in biomass conversion to fuels, chemicals, and materials via chemical and enzymatic routes.

Biochemistry labs [email protected]










Michael Reznikov, PhD

Principal Scientist, Electrodynamics

Physical Optics Corporation

Pulp and slurry dewatering, reduction of viscosity, electrospray, and electrospinning

Brookfield AMETEX XDV3T Rheometer; Beckman Coulter DEKSAMAX PRO particle sizing and Zeta potential analyzer; Resodyn LabRAM II (up to 1 kg payload) resonant acoustic mixer for solids, liquids, slurries, and high viscosity pastes, acoustic mixer; customized and upgraded electrospray and electrospinning station with DC (both polarities) and AC function generator (pulses, sin, triangle) high-voltage (up to 20 kV) sources, customized (internal web trail) technological oil-less vacuum chamber.

[email protected]





Nathalie Lavoine Assistant Professor

NCSU, Department of Forest Biomaterials, College of Natural Resources

CNF/CNC production and characterization; chemical surface modification (TEMPO, silanization, etc); foams (dry and wet)/aerogels; nanocomposites; (active) packaging materials; insulation materials; interfacial and colloidal sciences; mass and heat transfer;

Lab Facilities for CNF and CNC productions (Masuko grinder, aqueous counter collision - the only one available in the USA, refiners - valley beater, PFI mills, Turrax, acid hydrolysis setup); surface properties characterization (dynamic light scattering; quartz microbalance; static/dynamic contact angle; zeta potential/conductometry; thermal AFM); pulp, paper/paperboard characterization techniques and lab- & pilot-scale equipment (from pulping to papermaking); Properties: structural (optical microscopy; BET; external access to SEM), chemical (GPC, HPLC, IR, UV, NMR; external access to XRD/TOF SIM), mechanical (tensile/compressive, stiffness, burst strength, DMA, etc), thermal (TGA, DSC), rheology, and barrier (air/oxygen/water vapor permeability, grease resistance).

[email protected]

Paul L. Latten Director R&D Southeast Nonwovens, Inc.

spray coating NFC on nonwoven fiber blends with fiberglass, ceramic, pulp, etc

lab and commercial scale wet lay nonwoven lines

[email protected]

Peter Ciesielski Principal Research Scientist

National Renewable Energy Lab

Enzymatic Production, characterization (TEM tomography, AFM), molecular modeling

NREL Biomass Surface Characterization Lab, In house super computer (Eagle), cellulase enzyme engineering

peter.ciesielski@nrel .gov

Raghuram Dhumpa, Ph.D.

Vice President Innovatech Engineering

Nanocellulose sheet formation for dermatological applications, polymer composites.

Machinery to develop custom nanocellulose prototypes for end-user.

[email protected]




mailto:peter.ciesielski@nrel

mailto:peter.ciesielski@nrel





Roland Gong, PhD Associate Professor

University of Wisconsin -Stevens Point

upscale nanocellulose application including but not limited, disperse and mix nano cellulose with other materials in aqueous form, coating nanocellulose mixture on a web.

A pilot scale paper machine, a pilot scale inline coater and laminator, and complete material testing lab.

[email protected]

Scott Sinquefield Sr. Research Engineer

Renewable Bioproducts Institute at GA Tech

Drying Pulping lab with digesters, wide variety of characterization facilities, Pfaudler glass lined reactor.

[email protected]

Sergiy Minko Professor University of Georgia

research on functionalization of NFC and NCC, and applications in functional materials

laboratory-scale setups for fabrication, functionalization and testing NC and NC-containing materials

[email protected]

Shanju Zhang, Ph.D.

Associate Professor

California Polytechnic State University at San Luis Obispo

Nanocellulose production, modification and applications

Lab facilities including homogenizer, centrifuge, mixer, Rheometer, DSC, TGA, DMA, FTIR, NMR, GPC, PLM, AFM, SEM, XRD

[email protected]

Siqun Wang, PhD Professor University of Tennessee

Nanocellulose/nanolignin/nano carbon dots production, applications in nanocomposites, aerogel, 3D printing, Superhydrophobic coating, super capacitor and composites

Most laboratory facilities for CNF/CNF production (homogenizer, 2 supercollider grinders), characterization (zetasizer, DSC/TGA, X-ray, AFM, NMR, SEM, 3D printers), physical property tests (Instron, nanoindentor, NanoDMA, DMA)

[email protected]

Soydan Ozcan R&D Staff Oak Ridge National Lab

Nanocellulose production, drying, composites applications, additive manufacturing applications

In conjunction with UMaine, nanocellulose production/fibrillation, surface treatment, spray drying, compounding, composite and additive manufacturing application capabilities.

[email protected]












Steven Winter, PhD

Sr. Project Manager

International Paper Co.

MFC production, dewatering, drying and physical property testing of wood-pulp fibers

Pilot line facilities for MFC production. Supporting material measurement laboratory for fiber quality analysis a handsheet property testing.

[email protected]

Sunkyu Park EJ Woody Rice Associate Professor

North Carolina State University

Cellulose characterization (crystallinity, pore), dissolving pulp production, cellulose derivatives

Most laboratory facilities for biomass characterization

[email protected]

World Nieh National Program Lead, Forest Products

USDA Forest Service R&D

international standards development, National initiatives and policy, technology and commercialization assessment, innovation

Forest Service wide R&D, interaction with federal agencies

[email protected]

Yulin Deng, PhD Professor Georgia Institute of Technology

Nanocellulose production, applications in dewatering, aerogel, 3D printing, soft electronics and composites

Most laboratory facilities for CNF/CNF production (NanoBee homogenizer, supercollider grinder), characterization (zetasizer, DSC/TGA, X-ray, NMR, SEM, 3D printers), physical property tests (Instron, DMA)

[email protected]

Blake Marshall

Technical Manager

US Department of Energy

Composite material systems

Manage R&D portfolio focused on Nanocellulosics

[email protected]








Appendix E - Rapid Fire Presentations

Name Organization Rapid Fire Presentation Title

Carson Meredith Georgia Institute of Technology

Engineering to enable utilization of bioproducts

Alexander Kraus GEA GEA equipment portfolio for nanocellulose production

J.Y. Zhu USDA Forest Service Forest Products Lab

Sustainable Production of Diversified Cellulose Nanomaterials Using Solid Acid Hydrolysis

Siqun Wang University of Tennessee

Biobased nano materials from lab to commercialization

Colleen Walker University of Maine Production and Use of Cellulose Nanofibers

Meisha Shofner Georgia Institute of Technology

Nanocellulose Related Research at the Renewable Bioproducts Institute

Kim Nelson GranBio From Biomass to BioPlus®: Tailored Nanocellulose Products for Numerous Markets

Eric Mintz Clark Atlanta University Preparation And Characterization Of Nanocomposites Incorporating Lignin Coated Cncs And Cnfs Fabricated By High Torque Melt Mixing Or Extrusion

Jack Miller Biobased Markets Overcoming the Challenges to Business Development

Anna Carlmark RISE – Research Institutes of Sweden

Nanocellulose on the go and the world’s strongest nanocellulose filaments

M. Celeste Iglesias

Auburn University Nanocellulose Research at the Forest Products Development Center, Auburn University

Douglas Fox American University Facile Approach to Simultaneously Tune Surface Energies and Water Uptake of Cellulose Nanomaterials

Richard Berry Celluforce Celluforce

Roland Gong University of Wisconsin – Stevens Point

Nanocellulose Film and Adhesives

Douglas Gardner University of Maine Spray dried nanocellulose as functional additive for thermoplastic composites

Yulin Deng Georgia Institute of Technology

CNC and CNF aerogels, films and 3D printing: a summary of my research

Sergiy Minko University of Georgia Sustainable applications of nanocellulose

Paul Albee P3N Technology Inc. Specializing in the development of Additive Concentrates for plastic Applications

Erkki Hellén VTT Re-dispersable nanocelluloses with foam drying

Shanju Zhang California Polytechnic State University at San Luis Obispo

Bio-Enabled Compatibilization of Cellulose Nanofibrils

Veikko Sajaniemi Pöyry Management Consulting

SIMPLE COST EFFECTIVE MFC FOR PAPERMAKING


Name Organization Rapid Fire Presentation Title

Paul Latten Southeast Nonwovens, Inc.

A fiber based materials development & manufacturing company

Nathalie Lavoine North Carolina State University

Understanding Nanocellulose Fundamentals for Development of High-Performance Tailored Materials

BGL LLC BGL LLC: Dewatering/Drying Solutions

Santosh Vijapur Faraday Technology FARADAYIC® ElectroDewatering of Cellulosic Nanomaterials

Dilpreet Bajwa North Dakota State University

Enhanced Technology for Drying and Dispersion of Cellulose Nanocrystals

David Cowles Valmet, formerly GL&V Micro-Fibrillated Cellulose (MFC) – Production & Application Update

Michael Reznikov Physical Optics Corporation

Dielectrophoretic Enhancement of Dewatering


Appendix F - References

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2 K.J. Ong et al. A 90-day dietary study withfibrillated cellulose in Sprague-Dawley rats. Toxicology Reports, Vol. 7, 2020, pages 174-182.

3 E.J. Foster et al. Current characterization methods for

cellulose nanomaterials. Chem. Soc. Rev., 2018, 47, 2609. 4Shimadzu Corporation, Solutions for Cellulose Nanomaterials Application Notebook First Edition: Feb.

2019. 5 J. Miller, biobased Markets, Nanocellulose: Packaging Applications and Markets, RISI, 2019 6 J. Miller, biobased Markets, Nanocellulose: Packaging Applications and Markets, RISI, 2019 7 Miller, J., Nanocellulose Challenges and Opportunities, End User Perspective, TAPPI, 2018. See

https://imisrise.tappi.org/TAPPI/Products/01/R/0101R352BUN.aspx [imisrise.tappi.org] 8 https://birlacarbon.com/birla-carbon-and-granbio-technologies-introduce-breakthrough-innovation-in-nanocellulose-dispersion-composite-ndctm-masterbatch/ 9 https://www.bbi-europe.eu/projects/exilva 10 https://www.pulpapernews.com/20190803/7281/imerys-signs-two-supply-agreements-paper-

producers?page=0%2C10 11 https://www.usendowment.org/u-s-endowment-for-forestry-and-communities-to-host-the-worlds-largest-

test-of-groundbreaking-concrete-infused-with-wood/ 12 Sinquefield, Scott, et.al. A Review of Nanocellulose Drying and Dewatering, Unpublished Manuscript,

Renewable Bioproducts Institute at GA Tech, Atlanta, GA, April 2019 13 Amini, E.; Tajvidi, M.; Bousfield, D. W.; Gardner, D. J.; Shaler, S. M., Dewatering behavior of a wood-

cellulose nanofibril particulate system. Scientific Reports 2019, 9, 14584. 14 Sethi, J.; Oksman, K.; Illikainen, M.; Sirviö, J. A., Sonication-assisted surface modification method to

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15 Wetterling, J.; Jonsson, S.; Mattsson, T.; Theliander, H., The influence of ionic strength on the electroassisted filtration of microcrystalline cellulose. Ind. Eng. Chem. Res. 2017, 56, 12789-12798.

16 Wetterling, J.; Sahlin, K.; Mattsson, T.; Westman, G.; Theliander, H., Electroosmotic dewatering of cellulose nanocrystals. Cellulose 2018, 25, 2321-2329.

17 Dimic-Misic, K.; Puisto, A.; Paltakari, J.; Alava, M.; Maloney, T., The influence of shear on the dewatering of high consistency nanofibrillated cellulose furnishes. Cellulose 2013, 20, 1853-1864.

18 Dimic-Misic, K.; Maloney, T.; Liu, G.; Gane, P., Micro nanofibrillated cellulose (MNFC) gel dewatering induced at ultralow-shear in presence of added colloidally-unstable particles. Cellulose 2017, 24, 1463-1481.

19 Dimic-Misic, K.; Maloney, T.; Gane, P., Effect of fibril length, aspect ratio and surface charge on ultralow shear-induced structuring in micro and nanofibrillated cellulose aqueous suspensions. Cellulose 2018, 25, 117-136.

20 Dimic-Misic, K.; Puisto, A.; Gane, P.; Nieminen, K.; Alava, M.; Paltakari, J.; Maloney, T., The role of MFC/NFC swelling in the rheological behavior and dewatering of high consistency furnishes. Cellulose 2013, 20, 2847-2861.

21 Rantanen, J.; Maloney, T. C., Consolidation and dewatering of a microfibrillated cellulose fiber composite paper in wet pressing. Eur. Polym. J. 2015, 68, 585-591.

22 Clayton, S. A.; Scholes, O. N.; Hoadley, A. F. A.; Wheeler, R. A.; McIntosh, M. J.; Huynh, D. Q., Dewatering of biomaterials by mechanical thermal expression. Drying Technol. 2006, 24, 819-834.

https://urldefense.proofpoint.com/v2/url?u=https-3A__imisrise.tappi.org_TAPPI_Products_01_R_0101R352BUN.aspx&d=DwMGaQ&c=dpn1WjMMQGUYKOlM1k1w3OIaMfTHNTwPoUrrILOsxvs&r=0HPjq7E2pvnL6VZcDpOZQPIGMqoxdXTQj89QS4Mpcqo&m=-XHdeVKZqhsMim9vlUr55wnjOBVLUpdibzD6o9p4VN0&s=NAv-Q3KHFIWl8fDs2QF2-cKaGjst93usUFy6Ew6EUks&e=

https://birlacarbon.com/birla-carbon-and-granbio-technologies-introduce-breakthrough-innovation-in-nanocellulose-dispersion-composite-ndctm-masterbatch/

https://birlacarbon.com/birla-carbon-and-granbio-technologies-introduce-breakthrough-innovation-in-nanocellulose-dispersion-composite-ndctm-masterbatch/


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25 Baez, C.; Considine, J.; Rowlands, R., Influence of drying restraint on physical and mechanical properties of nanofibrillated cellulose films. Cellulose 2014, 21, 347-356.

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27 Peng, Y.; Han, Y.; Gardner, D. J., Spray-drying cellulose nanofibrils: Effect of drying process parameters on particle morphology and size distribution. Wood Fiber Sci. 2012, 44, 448-461.

28 Peng, Y.; Gardner, D. J.; Han, Y.; Kiziltas, A.; Cai, Z.; Tshabalala, M. A., Influence of drying method on the material properties of nanocellulose I: thermostability and crystallinity. Cellulose 2013, 20, 2379-2392.

29 Aguiar-Ricardo, A., Building dry powder formulations using supercritical CO2 spray drying. Curr. Opin. Green Sustain. Chem. 2017, 5, 12-16.

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31 Voronova, M. I.; Zakharov, A. G.; Kuznetsov, O. Y.; Surov, O. V., The effect of drying technique of nanocellulose dispersions on properties of dried materials. Mater. Lett. 2012, 68, 164-167.

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33 Wang, X.; Zhang, Y.; Jiang, H.; Song, Y.; Zhou, Z.; Zhao, H., Fabrication and characterization of nano-cellulose aerogels via supercritical CO2 drying technology. Mater. Lett. 2016, 183, 179-182.

34 Khoshkava, V.; Kamal, M., Effect of drying conditions on cellulose nanocrystal (CNC) agglomerate porosity and dispersibility in polymer nanocomposites. Powder Technol. 2014, 261, 288-298.

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41 Khoshkava, V.; Kamal, M. R., Effect of drying conditions on cellulose nanocrystal (CNC) agglomerate porosity and dispersibility in polymer nanocomposites. Powder Technology 2014, 261, 288-298.

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43 Farahbakhsh, N.; Roodposhti, P. S.; Ayoub, A.; Venditti, R. A.; Jur, J. S., Melt extrusion of polyethylene

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45 Raquez, J. M.; Murena, Y.; Goffin, A. L.; Habibi, Y.; Ruelle, B.; DeBuyl, F.; Dubois, P., Surface-modification of cellulose nanowhiskers and their use as nanoreinforcers into polylactide: A sustainably-integrated approach. Composites Science and Technology 2012, 72 (5), 544-549.

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49 Gupta, A.; Simmons, W.; Schueneman, G. T.; Hylton, D.; Mintz, E. A., Rheological and Thermo-Mechanical Properties of Poly(lactic acid)/Lignin-Coated Cellulose Nanocrystal Composites. Acs Sustainable Chemistry & Engineering 2017, 5 (2), 1711-1720.

50 Herrera, N.; Salaberria, A. M.; Mathew, A. P.; Oksman, K., Plasticized polylactic acid nanocomposite films with cellulose and chitin nanocrystals prepared using extrusion and compression molding with two cooling rates: Effects on mechanical, thermal and optical properties. Composites Part a-Applied Science and Manufacturing 2016, 83, 89-97.

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