CO2 Sequestration: Processes and Methodologies...CCS Technologies ..... 15 Cryogenic Process ........

CO2 Sequestration: Processes andMethodologies

Chandra Sekhar Kuppan and Murthy Chavali

ContentsIntroduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 3Emission Reduction Policies and Status of Countries . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 5Models and Predictions . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 7Effect of CO2 Increase . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 8Carbon Dioxide Removal (CDR) Approach . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 9

Bioenergy with Carbon Capture and Sequestration (BECCS) . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 9Direct Air Capture and Sequestration (DACS) . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 10Afforestation and Reforestation . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 10Soil Carbon Sequestration . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 10Enhanced Weathering . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 10Ocean Fertilization . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 11

Carbon Capture and Sequestration (CCS) Technologies . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 12Different Types of CCS . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 13CCS Technologies . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 15Cryogenic Process . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 28

Sequestration of Captured CO2 . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 29Geological Sequestration of Carbon Dioxide . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 29

Value Added Application of CO2 . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 31Albedo Modification . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 33Future Perspectives and Conclusion . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 34References . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 35

C. S. KuppanDivision of Chemistry, VFSTR University, Guntur, AP, India

M. Chavali (*)Shree Velagapudi Rama Krishna Memorial College (PG Studies), NAAC ‘A’ Grade & ISO9001:2015 Certified (Autonomous), Guntur District, Andhra Pradesh, India

MCETRC, Tenali, Guntur, Andhra Pradesh, Indiae-mail: [email protected]

# Springer Nature Switzerland AG 2019L. M. T. Martínez et al. (eds.), Handbook of Ecomaterials,https://doi.org/10.1007/978-3-319-48281-1_6-2

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AbstractRapidly growing economy and its consequence of relying heavily on the fossilfuels, for power generation, accounts for the major CO2 pollutant in the atmo-sphere. Natural carbon cycle process will not be effective in reducing the pollut-ant content, as the amount and rate of CO2 dissipation raise at a drastic rate. Thisalarming situation urgently requires technologies for carbon dioxide capture andsequestering (CCS). With the development of technologies every day, the amountof CO2 emission is expected to increase steeply, which necessitates more tech-nologies to sequester CO2 with a target of 50 ppm by 2050. CCS involves thecapture of gas at some stage of the industrial process followed by pressurizationand transporting it to stable geological sites like saline aquifers, depleted oil andgas fields, deep coal seams where it can be trapped for thousands of years. CO2

sequestration requires multiple fundamental R&D approaches and significantbreakthroughs. The purpose of this review is to have an integrated analysis ofthe carbon sequestration process including the state of the art technologies forCO2 capture, separation, transport, storage, leakage, monitoring, and life cycleanalysis.

Depending on the source of emission, different techniques and methodologiesadopted by the scientific community were analyzed and discussed. A briefdescription of the best practices and techniques for CO2 capturing like absorption,adsorption, cryogenic, and membranes will be reviewed. A comparative study onthe same will be analyzed based on their performance, efficiency, regeneration,adsorption rate, the volume of adsorption, cost, and energy required for regener-ation. Some of the prerequisites for sequestering the captured carbon dioxide aresafety, environmentally benign, effective, economical, and acceptable to thepublic. Natural sequestration methods include plantation, soil carbon sequestra-tion, and CH4-CO2 reforming. Industrially acceptable sequestration processinvolves isolating the captured gas into places which are nonaccessible to livingcreatures which include basically geologic, oceanic, and terrestrial dumping sites.All the three geoengineering techniques and their subdivisions will be discussedin detail with up to date improvisations and results. Moreover, the concernsrelated to potential leakages while transporting supercritical CO2, uncertainty interms of quantification of storage potential, accompanied by monitoring andengineering challenges have to be given prior attention in developing any seques-tration process, which this review will give an overall picture and suggestions.

KeywordsCarbon dioxide capture sequestration (CCS) · Carbon cycle · Oxy-fuelcombustion · Paris agreement · Greenhouse gas · International Panel on ClimateChange (IPCC) · Negative Emission Technology (NET) · Bioenergy with carboncapture and storage (BECCS) · Afforestation and reforestation (AR) · Direct aircapture and storage (DAC) · Soil carbon sequestration (SCS) · Enhancedweathering (EW) · Ocean fertilization (OF) · Silicate weathering · Ironfertilization · Chemical looping combustion (CLC) · Precombustion ·

2 C. S. Kuppan and M. Chavali

Postcombustion · Carbamate · Metal oxide frameworks (MOF) · Membranes ·Carbonaceous material · Polyethyleneimine(PEI) · Metal oxide · Cryogenicprocess · Geological sequestration · Albedo modification

Introduction

The new millennium in the second decade started with industrialization in every partof the world improvised the livingness of humans in one end but at the receiving end,the atmosphere got polluted by these industrialization strategies by dumping dan-gerous greenhouse gases. This was not noticed until a catastrophe happened in theform of depletion of ozone over the earth’s crust. Increased energy demand from allsectors of civilization including anthropogenic release has led to an increase in fossilfuel consumption, releasing large amounts of gases such as CO2 into the atmosphere.Still one of the common fuels used in most of the industrial processes is coal.

The pollutants that have been dumped into the atmosphere for human livingnessin the name of civilization were called as anthropogenic pollutants, which can be inany form (solid, liquid, or gas), but the one which notoriously increased unnoticedwas gaseous pollutants. Greenhouse gases include CO2, CH4, SOx, nitrous oxide,water vapor, ozone, and perfluorocarbons/chlorofluorocarbons [1]. Though green-house gases like methane, chlorofluorocarbons have serious effects on the atmo-spheric climatic conditions, CO2 has the potential to leave permanent damage to theatmosphere and its percentage is high and is responsible for 70% of the greenhouseeffect leading to global warming. CO2 contributed to 84% of greenhouse gas in theUSA in 2000 all due to increase in emission rate since the industrialization from1800. A total of 97% of this is due to anthropogenic CO2 emission, attributed tofossil fuel contribution such as power plants, incineration, and motor vehicles. Othersources are cement, lime, and iron/steel manufacturing units. And 60% of the globalgreenhouse gases contribute to global warming [2] which can be seen from a100 ppm increase of CO2 content from preindustrial level.

CO2 emission is not only anthropogenic; it is released by natural sources also likesoil, oceans, plants, animals, and volcanoes [3]: 42.8% was released by oceans,around 28.5% by plants and animals respiration [4], 28.5% by soil respiration anddecomposition, and very little percentage of 0.03 by volcanic eruption [5, 6] as givenin Fig. 1.

Though the anthropogenic source of CO2 was smaller when compared to thenatural emission, that amount is more than enough to upset the natural balance ofcarbon cycle which existed prior to the industrial era. Existence of natural sink is thereason for maintaining the balance of CO2 in the atmosphere, which gets disturbedboth positive and negative ways with excess of greenhouse gas pushed into theatmosphere because of human activities [7] such as burning of fossil fuels (87%),deforestation (9%), and industrial processes (4%) as given in Fig. 2a. The types offossil fuels [8] (Fig. 2b.) used commonly are coal (43%), natural gas (36%) and oil(20%).For every ton of fuel burned, around 2.5 ton of CO2 will be released [9]. Theelectricity sector is the major contributor among them consuming around 60–90% of

CO2 Sequestration: Processes and Methodologies 3

fuel globally, with the exception of Canada and France, which relies on other sourcesof power generation like wind, hydro, solar, etc. Industry relies upon this electricityto 92% for manufacturing chemicals, cement, aluminum, iron/steel, paper produc-tion, etc. The rest of the electricity is used for the residential and commercial sectorsfor lightning, heating, and running electrical appliances (Fig. 2c.). The transportsector is the second largest user of fossil fuels to release CO2 into the atmosphere.This sector is growing every year as the purchase of vehicles increases despite anincrease in the crude oil price. Since 1990, it is found that a rapid growth of 45% wasobserved in less than 2 decades of time. Road transport (Fig. 2d.) accounts for 72%,marine shipping accounts for 14%, and the global aviation sector the remaining 11%

Ocean42.87%Plants & Animal

respiration28.55%

Soil respiration&

Decomposition28.55%

Volcaniceruption

0.03%

Natural source of CO2

Fig. 1 Different sources of CO2 by natural phenomena

Natural gas36%

Oil20% Coal

44%

Aviation11%

Marine15%

Industry92%

Fossil fuel87%

Industrialprocess

4%

Anthrophogenic event Fossil fuel

TransportElectricity

a b

c d

Deforestation9%

Household/commercialapplication

8%

Road74%

Fig. 2 (a) Different anthropogenic sources, (b) different types of fossil fuels, (c) usage ofelectricity in different sectors, (d) different types of transport accounting for CO2 emission


[10]. When compared to the number of ships and vehicles, the number might be lessfor ships or marines, but the pollution is most nasty because the fuel used is not arefined petroleum product, which is about 1 billion ton of CO2 emission [11].

Simulation studies on global warming predict an increase in average globaltemperature and sea levels, shifts in weather patterns and more extreme weatherevents, including flooding and droughts. Though CO2 is mostly a diluent with no fuelvalue, it is acidic in nature and may cause corrosion problems in the presence of watercreating carbonic acid which will be corrosive to metals and alloys. The major effectof global warming includes sea level rise, change in ocean acidity, increase in violentweather phenomena, stress on wild life and ecosystem, and a new environmentalcondition which affects food security, harm humans, settlement, and infrastructure.The consequence of this anthropogenic source to the environment has to be conveyedto all, who utilize fossil fuel for their living with the knowledge of the effects causeddue to these gases, which makes it much easier for the lay man to understand or relatethe effects and change the way he lives to reduce the climatic effect.

Once the need for CO2 capture and sequestration was made inevitable, a hugeamount of projects were proposed, worked, and put forth for industrial and com-mercial usage. Many reviews/articles were published and kept open to all under thetopic [12–16]. Some of the technologies were not open to the research community,which was protected under the international patenting act. In that scenario, very fewpublications talk about the current status of patents on CO2 capture [17]. Hugevolumes of patents were filed till date, and this number shows the seriousness of theongoing climatic issue and the number of active research going on globally tocontrol the global warming in a way or two.

This chapter will discuss first the present status of signed agreement/promises bydifferent countries towards reducing CO2 emission followed by different simulationstudies. Various mitigating approaches to reduce the CO2 emission under carbondioxide removal (CDR) both directly and indirectly from the atmosphere werediscussed. Different carbon dioxide capturing and sequestration (CCS) processtechniques were reviewed, which were designed to stop emission of CO2 to theatmosphere by the industries. CCS techniques under precombustion, post-combustion, and oxy fuel combustion were discussed in detail for capturing thereleased gas and concentrating it. Before sequestering the captured CO2 different theamenable ways of utilizing were discussed as that too accounts for removing the CO2

from the atmosphere. Sequestration under geological sites, troubles in using the sites,and advantages and disadvantages are discussed. A new approach called albedo,with its advantages and disadvantages, to reduce global warming, was discussedalong with the future scope to mitigate CO2 emission.

Emission Reduction Policies and Status of Countries

Kyoto protocol in 1997 was the first major initiative taken towards the ill treatmentof our environment. Kyoto protocol is aimed to reduce the CO2 emission and for thisnumerous nations have committed to the cause along with controlling other


greenhouse gas emission. Kyoto protocol urged 37 industrialized countries and theEuropean Union to reduce its greenhouse gas emission on an average to 5.7% from1990 during the period of 2008 to 2012. Copenhagen Accords request to the globalnations is to contain the global temperature to 2 �C above the preindustrial era by2100 [18, 19].

In 2015 December, a new global agreement to combat climate change under theUnited Nations framework convention on climate change (UNFCCC) was signed bycountries that had an intention to reduce the climatic changes. In continuation of this, allthe countries gave plans to address the climate change challenge after 2020. TheIntended Nationally Determined Contribution (INDC) addresses a range of issues,which can relate to avoid, adapt, or cope up with climate change, among other things.Until now the decisions made by INDC are not final and can be modified up until thetime Paris agreement signed in 2015 was ratified. For now, they represent a betterunderstandingof the actions by the countrieswho have intended to pursue the agreementafter 2020 toward reducing global warming. So the ultimate goal of other steps is toreduce the average global temperature to 2 �C below the preindustrial era and tomaintain the temperature increase to 1.5 �C above preindustrial levels. This level wasfixed by the committee keeping inmind that the level will not pose danger to the climaticcondition while ensuring sustainable production and economic development.

The prediction by the International panel of climate change (IPCC) for the year2100 (a) will show an increase in the atmospheric CO2 level of 570ppmv, (b) the seawill rise its level about 3.8 m, and (c) the temperature will increase about 2 �C[20–24]. Till now, as per the 5th assessment report (AR5) by the IPCC, there are 116scenarios that are consistent with a >66% probability of limiting the global temper-ature to <2 �C, which is equivalent to 430–480 ppm of CO2 equivalents by 2100.

The recently concluded July 2017 Paris agreement meet is to have a review andknow the status of the policies imposed by the 153 countries to mitigate thegreenhouse gas emission. This is in a way rebooting the climate policy and givesflexibility to those countries to stick on to the signed policy. An article was recentlypublished in nature [25], stating the current state or scenario of the Paris agreement2015. The article focused on the importance of the agreement, the effect of with-drawing from the treaty by the USA, and problems faced by Europe, Japan, SouthKorea, and Australia to mitigate the promised CO2 cut. Political issues and theprojected reduction if the agreement goes not as intended.

The top six countries that are responsible for about 60% global CO2 emission areChina [26], USA, India, Russia, Japan, and Germany. China accounts for 30% of theemission which is twice the amount of greenhouse gas emitted by the USA. A dealsigned by China and USA to stem down the greenhouse gas emission growth by2030 is the major step taken by China towards global warming, though it will notcombat the full emission because China relies on fossil fuel for electricity and steelproduction and being the top developing country, it demands more industrializationwhich keeps them on the top of the table.

The USA under Obama’s administration pledged to cut the emission to 26–28%below 2005 by the year 2015. But till now it has achieved around 15–19% whichwas made possible by shifting from coal to natural gas for power generation [27].


The USAwith the deal with China promised to double the speed of process to reduceemission by losing the carbon pollution 26% by 28% from 2005 level by 2025.Despite the USAwithdrawing from 2015 Paris agreement in 2017, the platform waslaid by the then Obama Government which will push the US economy towards cleanenergy but at a slower pace than before.

Japan has promised to reduce the emission to around 25% by 2030, which theywanted to achieve through their efficient economy system by installing a devicewhich can utilize around 40% of less energy in all new equipment’s. From theelectricity sector, Japan has planned to get the power of about 20–30% using carbon-free nuclear plants, by 2030, but only 15% is possible in the current scenario. Toinitiate this initiative, Japan has already closed more of its reactors and currently,only 5 plants are operational among the existing 42 plants [28]. From 2012, theyhave started carbon taxing based on the emission of fossil fuels, with the aim to moveto renewable energy and energy saving projects.

The European Union struggles to keep the promise. EU has planned to cut shortits power and industrial sectors emission to ~43% below 2005 levels by 2030. This isexpected to be achieved by switching from coal to gas as the USA, rather thanconstructing new renewable energy or nuclear plants or carbon capture and storagefacilities [29]. The remaining ~55% contribution is from buildings, transport, agri-culture, and waste which is not possible to reduce without the implemented policies.

When the Kyoto protocol in 1997 was amended, Russia was not on the list for amoderate cut in emission. But the scenario changed after the Soviet Union collapsed.Being a major player in oil and gas production, Russia announced in 2013 a targetcut of 25% from 1990 levels by 2030, but the average CO2 emission was already35% less than its 1990 levels.

Indian scenario is an interesting one, because of its blooming population andeconomy it will put them in an increasing trend of CO2 emission. Another importanthappening is that India has signed voluntarily in 2010 to reduce the CO2 emission by20–25%which is well above its pace and standard with respect to its economic outputby 2020. CO2 emission as per 2000 survey in India was 956Mt (million tons) for aperiod of 1 year (1999–2000). The sector which is responsible for thismuch amount ofCO2 release was from thermal power plants, steel plants, cement plants, fertilizerplants, refineries, and petrochemical plants, which contributed to around 64% ofoverall India’s emission. The survey that conduced in 2004 for CO2 emission inIndia was totally 1343Mt, in this the large point sources contribution was 53.7%which is lesser than the emission when compared to 2000 statistics which is a positiveapproach towards global CO2 reduction [30]. Onemajor attempt is to install solar gridswhich are expected to increase the power generation five-folds to 100 Gwh by 2030.

Models and Predictions

The climatic change expected to be flourishing in the future due to the greenhousegases was projected by many agencies and departments. All these private/govern-ment/NGOs which are keenly following the changes use certain models which give a


comprehensive data by taking into consideration the global carbon cycle. Oneproject which gives a collective data of about 11 models is coupled carbon cycleclimate model intercomparison project (c4MIP). Anonymously all these modelsprojected an increase in future atmospheric CO2 concentration. Despite this, allmodels showed a disparity in the magnitude of the effects, which might result dueto some uncertainty in the parameters for calculation. Improvisation over C4MIPmodel was done by simulating the process over a prescribed concentration of CO2.This model was recommended by Hibbard et al. as the experimental design for phase5 of the coupled model inter comparison project (CMIP5). The latest state-of-the-artearth system general circulation models (ES-GCMs) have recently been used tocarry out simulation for a new set of scenarios for CMIP5. One among this scenariowill be computed in such a way the concentration of CO2 pathway was similar to theanthropogenic emission by 4 integrated assessment method (IAM) [31]. Based onthe predicted emission level at 2100, representative concentration pathway wasarranged from 421, 535, 670, and 936 ppm. IAM’s estimate of further emissionactivities including land usage was also included in the calculation, which was notincluded in the ES-GCM package with varying complexities in scenarios andconditions.

Effect of CO2 Increase

Emission of anthropogenic greenhouse gas CO2 to the atmosphere has raised greatconcerns towards global warming, which broadly contributes to acid rain, smog, andhealth issues. Greenhouse gases threaten public health and the environment/scienceoverwhelmingly shows greenhouse gas concentrations at unprecedented levels dueto human activity [32]. The annual uptake of CO2 by plants through photosynthesisas carbon cycle was around 25% which is equivalent to around 200billion tons ofcarbon, but the alarming thing is around 195 billion tons is once again released intothe atmosphere through human respiration and ocean outgassing. The decrease in the14C/C ratio in tree rings is one way of assessing the increase in CO2 concentration inthe atmosphere which was used for plant photosynthesis [33].

Dissolution of CO2 will produce hydrogen ions and makes the ocean water moreacidic and disturbs the marine life. Marine ecosystems are sensitive to temperatureand ocean acidity. A temperature increase might increase the carbon uptake by thephytoplankton by photosynthesis, but the adverse effect happens to their counterpartmarine organisms. They feel the heat stress and due to increase in acidity, the coralsget bleached off showing the white carbonate shell. This bleaching action will lead tothe starving of the corals [34, 35]. So because of the climate change, certain specieswill be forced to adapt to the changing climate or some will be forced to change theirmigration pattern or certain exotic species might end up with extinction [36, 37].

Food production will also face a serious problem. Although the relationship iscomplex, some regions will experience longer growing seasons, while others willsuffer from more heat stress where the global yields of wheat, barley, and maize havealready been decreased by increasing global average temperature [38].


Shifts in mean temperature, temperature variability, and precipitation patterns arealready causing stress on a diversity of ecosystems [39]. Species’ range shifts havealready become evident [40–44] and are expected to accelerate with increasing ratesof climate change, as a change in the timing of species migrations [45] and otherimportant plant and animal life-cycle events. There are many climatic adaptation andresilience efforts ongoing within the United States, often at the state or local levels[46]. Although this is a rapidly evolving field, there is still a great deal of research tobe done in the field of climate adaptation and there may be insufficient capacity foradaptation [47]. Overall, both humans and ecosystems face substantial challenges inadapting to the varied impacts of climate change over the coming century. Precip-itation patterns, unusual seasonal migration of species [45], variable life cycle eventsin plants, and animals might increase with increasing rate of climate changes [39].

Carbon Dioxide Removal (CDR) Approach

Actions that are responsible in enhancing the reduction of natural emission orincrease the natural CO2 removal will have the potential to lower the atmosphericCO2 content. Most of the major approaches for reducing the CO2 concentrationinvolve capturing from the atmosphere, concentrating and disposing it at remotelocations. Some of the negative emission technologies (NET) [48, 53] under CDRapproach are bio energy with carbon capture and storage [54, 55] (BECCS), Affor-estation and Reforestation [56–58] (forest management) (AR), Direct Air Captureand Storage [59, 60](DAC), Soil Carbon Sequestration [61–64] (SCS), EnhancedWeathering [65–68](EW), and Ocean Fertilization [69–71] (OF). In general thepotential for BECCS, AR, and DAC is high and for EW, SCS, and OF is lowcomparatively. All these processes might work in small scale but on implementationin large scale have serious drawbacks.

Bioenergy with Carbon Capture and Sequestration (BECCS)

Extraction of energy from biomass by oxidizing and in situ capturing of theproduced CO2 is called as bioenergy with carbon capture and sequestration(BECCS). The main source for BECCS is the biomass, which assimilates theatmospheric CO2 via photosynthesis. This biomass is then used to generate energyat the expense of liberating CO2 and water vapor. Biomass can also be used to getbiofuels such as ethanol, methanol, hydrogen, which will not cause net sequestrationof carbon but will involve in the production of energy and subsequent emission ofCO2 back to the atmosphere. Literature estimates a bioenergy potential in the rangeof 50–675EJ/year [72]. Large-scale deployment of BECCS has risks associated withit, but it is still not the right time to implement the process as this will not bring inbenefit to the climate. There won’t be any substantial net difference in carbonemission prior to the point where the CCS is tried to fossil fuel.


Direct Air Capture and Sequestration (DACS)

DAC is a chemical process where synthetic sorbents are used to capture atmosphericCO2 directly. The sorbents are in the form of amines, alkali/alkaline earth metaloxides, polymers, etc., which will be regenerated. It is a process in which theatmospheric CO2 is directly removed by using scrubbers and produces concentratedCO2 as the end product which will be sequestered or used for other purposes. Thescrubbing process can be by either adsorption or absorption or both or throughmembranes, etc. The CCS process and DACS might have similarities in separationprocess, but they differ in the point source, as CCS point sources like coal firedpower plants, chemical plants, etc., have a concentration much higher than the pointsource of DACS which separates from a very dilute atmospheric source (100–300times less than the flue gas). This dilution requires more energy for the separationprocess which will be around 2–10 times higher than the point source capture. Forthis reason, DACS process was slightly expensive than the CCS process.

Afforestation and Reforestation

AR is part of the natural carbon cycle where the released CO2 is captured by theplant’s trees to convert them to O2 and store in living biomass. It is reported that byimplementing global reforestation and afforestation, it is possible to remove around1Gt CO2 per year because forests are part of the natural sinks to curb CO2 fromatmosphere directly [73].

Soil Carbon Sequestration

Soil carbon content is expected to fall down by 25–50% after a period of 30–50 yearsfrom now due to intensive soil cultivation [74–76]. The soil carbon content can beimproved by growing cover crops, leaving the residues to decay in the fields,applying compost manures, and double cropping and other land management tech-niques to increase the soil structure and organic matter inputs. Bio char is onepotential technique to fix the carbon content in the soil. Bio char is a unique processwhere the biomass is pyrolyzed to become a product which is more resistant todecomposition, which when added to the soil can store the embedded carbon and insome cases enhance fertility.

Enhanced Weathering

Enhanced weathering involves grinding and spreading of rocks to increase theirsurface area so that it absorbs CO2 more rapidly and efficiently. The ground rock canbe spread on land or on the ocean to absorb atmospheric CO2. Accelerating orinducing the active solid rock materials to remove atmospheric CO2 is a new


approach for EW. The CO2 released in the atmosphere gets converted to bicarbonateions when it dissolves in the ocean, which settles at the bottom of the sea floor [77].This natural process can be utilized successfully for CO2 removal process, byaccelerating the reactions by bringing CO2 in contact with a natural rock formation,where the carbonate will be formed insitu [78–80]. All these weathering processesoccur in a timescale of few seconds to millennia. An advantage of this process isassociated with the acidity caused by the gas. The acidified ocean or sea afterdissolving CO2 will naturally resist further dissolution of CO2. But the dissolutionof carbonate salts of calcium will neutralize the acidity and allows the sea to dissolvemore CO2 [81]. The calcium carbonate added to ocean reacts with water and CO2 toform calcium and bicarbonate ions. These are the ions which increase the alkalinityof the ocean and neutralize the acidity and balance the pH of the water.

CO2 þ CaCO3 þ H2O ! Ca2þ þ 2HCO3�Speeding this process will be a potential technique to reduce the CO2. Silicate

weathering [82–84] does the same conversion of CO2 to bicarbonate, but here it willbe by using calcium silicate

2CO2 þ CaSiO3 þ H2O ! Ca2 þ 2HCO3� þ SiO2

Silicate weathering consumes two moles of CO2 compared to calciumweathering. The issue here will be the raw material for the weathering, and it requireslarge quantities of calcium carbonate, ~2.3 times larger than the mass of CO2

removed.

Ocean Fertilization

Phytoplankton’s and microscopic plants are some of nature’s gift, which can con-sume the CO2 from the ocean surface and convert them to organic matters, which canbe consumed by other marine habitats or its will settle at the deep of the ocean. Thesuccess of this approach will depend on a number of nutrients (nitrogen andphosphorus) present on the ocean surface and the rate of utilization of these nutrientsby the phytoplankton. So fertilizing the ocean surface with nutrients containingnitrate and phosphates will increase the growth of phytoplankton and ultimately itwill sequester the CO2 under the ocean bed. Compared to nitrogen and phosphorusfertilization, iron fertilization is more practical. The reason is the organic matter inthe planktons has a lower ratio of carbon to nitrogenous phosphorous than the ratioof carbon to iron (1000 to more than 10,000 on a mole/mole basis) [85]. It wasexperimentally proved that a small scale release of iron to high nitrate and lowchlorophyll content lead to increased phytoplankton growth rate [85, 86]. Likeanother process, iron fertilization too has environmental concerns to look into beforeimplementing. Projected Data on different CDR process for the year 2100 are givenin Table 1.


The potential benefit of any CDR process has to be estimated by the methodsfeasible capacity to remove the atmospheric CO2 over a timescale of interest. Asmentioned earlier, these CDR process will give a measurable effect only after thedepletion of fossil fuel. Until then these processes will cannot be implemented fully.

Carbon Capture and Sequestration (CCS) Technologies

The concluding remarks of 2015 Paris agreement were to reduce the climatictemperature or global warming to a level of �2 �C when compared to the pre-industrial era or at least �1.5 �C. The negative sign itself implicates how bad theatmosphere has been polluted, which means even if we stop all the anthropogenicrelease of CO2now, which will not decrease the global warming. To bring to acontrol, the temperature has to be dropped �1.5 �C which is only possible throughmitigating processes to scrub the CO2 released along with natural carbon cycleprocess. A simple relationship was developed in the name of modified Kaya’sidentity [89], which gives the relation between the amount of CO2 emitted to theenergy produced by carbon-based fuels considering the economy, population, andnatural sink.

CD ¼ PGDP

P

� �E

GDP

� �C

E

� �� SCO2

where CD is the CO2 emitted, P is population, GDP is a gross domestic product interms of economic development, E is over all energy production, C is the amount ofenergy produced by using carbon-based fuels, and SCO2 is the amount of CO2

consumed by the natural sinks. Interesting information we can derive from thisrelation is the possible ways by which the emission can be minimized or stopped.One way is to increase the natural and artificial sinks to absorb the emitted CO2, byplanting more trees, making artificial lakes and ponds with the marine eco systemalong with CCS techniques. Another way is to increase the usage of renewableenergy like wind, solar, hydro, and nuclear energy. One more option will be toreduce the usage of energy or conserve energy where the E/GDP factor will increasebecause the GDP will go down. All these three ways are feasible to reduce theemission.

Table 1 Projected Data on different CDR process for the year 2100 [87, 88]

CDR Approach 2100 potential (GtCO2/y)

BECCS 3.67–12.1

AR 4.03–12.1

DAC 3.67–12.1

SCS 1.47–2.57

EW 0.73–3.67


Carbon capture and storage refers to the set of technologies developed andimplemented in order to capture the parasitic CO2 gas in the atmosphere releasedby all sources including industries, power sectors, anthropogenic, etc., followed byhandling the gas and transporting it and storing in a place which will not release thegas to the atmosphere once again, for example, injection and storage in deepgeological formations. CCS will contribute to 1/6th of CO2 emission reductionrequired in 2050 and 14% of cumulative emission reduction between 2015 and2050 when compared to business as usual which will elevate the average globaltemperature by 6 �C. The overall application of CCS will totally depend on thematurity of the process, its cost, its potential and efficiency, and the ease oftransferring the technology to developing countries for process implementationrelating to regulatory aspects, environmental issues, and public’s perception.

Different Types of CCS

Some of the well developed and about to commercialize technologies for CCS are:

1. Precombustion removal of CO2 from the fuel.2. Postcombustion removal of CO2 from flue gas.3. Oxy-fuel combustion (OFC) by concentrating the CO2.4. Chemical looping.5. Clathrate hydrate process.

Currently, various CO2 capture technologies exist including physical adsorption[90–98]. However, they are still far from being considered as a technologicallyviable solution for scale-up options. The obvious bottle necks are the huge amountof flue gas which needs to be treated as well as low mass transfer rate during theprocess. Among the various principles, adsorption process seems to be available onewith minimum limitations and less energy consumption. An overview of differenttechniques under CSS process is shown in Fig. 3. To overcome the limitations, theprocesses were modified and improvised using both the principles of adsorption/absorption by using a solid porous substrate, which makes the regeneration processsimple and at a lesser energy cost. Chemical adsorption or physical adsorbents bothshould have some criteria’s to be used in CC technology, for example, the adsorbentsshould have high reactivity to the incoming stream of gas, selectivity, low vaporpressure, easy regeneration, and high thermal and chemical stability, and all of thisshould be economically viable to be used in industry scale.

The precombustion process uses carbon in the fuel to get converted to synthesisgas by combusting. The resulting gas can be further converted into a stream of highlyflammable H2 and CO2 using integrated coal gasification combined cycle (IGCC).This stream is separated for CO2 and stored. This technology is in the matured stateand it requires more capital cost for full implementation in industries. In thepostcombustion technologies, the CO2 will be in the dilute state (10–15%), whichrequires concentrator and adds on to the capital cost with an additional energy


requirement for the plant operation (20–30%). Oxy-fuel is the technique which isunder process for commercialization, and the advantage with this process is it can beoperated at high pressures, but the drawbacks will be using expensive cryogenicunits for air separation.

In all these cases, the main factors which are inhibiting the efficiencies of the CCtechniques are the concentration and composition of flue gas, its operational tem-perature, and the excess energy requirement for the desorption processes. Among thedifferent process mentioned above, precombustion technology is the most econom-ical, thermodynamically and kinetically attractive as it will feed a high concentrationof CO2 with high pressure for CCS. Postcombustion process is the advantagesprocess despite its expensiveness, and it can be integrated with the respective plantsto increase its efficiency simultaneously. Postcombustion process has differenttechniques like adsorption, absorption, membrane technology, and separationusing cryogenics. Adsorption can be either chemically or physically interactingwith the adsorbed gas, where the physically adsorbed process will be the easierand convenient technique to retrieve the adsorbed gas. The chemically adsorbedtechnique has the advantage of working even at low pressure and low concentration

Fig. 3 Overview of different techniques under CSS process


conditions with high selectivities. All the available approaches for CO2 reduction arediscussed in the following section (see Fig. 4).

CCS Technologies

AbsorptionThe absorption techniques are the most commonly used techniques to remove theatmospheric CO2, but due to the low solubility of a gas in the absorbent, theefficiency is reduced as the rate determining factor is the mass transfer of CO2 intothe liquid side. The mass transfer rate can be improved apart from functionalizationby incorporating or blending the absorbent with solid adsorbents [99–103]. One suchsolid adsorbent is activated carbon. For an adsorbent to be efficient, it should possesstwo qualities [100–102, 104, 105]: hydrophobicity enough to self- assemble at theinterface of air/liquid for better adsorption and competitiveness for adsorptiontowards higher adsorption capacity by having higher surface areas. Many reportshave been published for different gas over different solid adsorbents; all were foundto be effective. Zeolites were hydrophobically modified for this study and it wasfound much efficient than the activated carbon system [106–108].

The process of using ammonia or amine solution, which uses the principle ofabsorption, was one among the above-said process, which was studied in detail. Thisprocess was comparatively mature, but it has got many disadvantages which stop itsuse for the long run.

Amine or Ammoniaþ Carbon dioxideþ water ! Ammonium Carbonate

or

Ammonium Bicarbonate

Fig. 4 Pictorial representation of the three CCS process


This reaction which traps the CO2 in the form of byproducts was not reversibleand hence it requires more energy to reverse CO2 and the recycling of amine orammonia for reuse becomes difficult. The used amine may affect the ecosystem aswell as the metallic machinery as amine is corrosive in nature.

Industrially, use and throw components are less desirable due to the addedexpense and maintenance associated with disposal of huge amounts of spent activematerial. Regenerative systems are designed to regenerate the active materialsmaking it suitable for a subsequent productive material for further use. The activescrubbing material for one of the process was calcium oxide and alkali metal ions.

Some of the existing commercial processes for physical absorption are Selexolprocess [109], Rectisol Process, Purisol Process, and Fluor process. Table 2 gives thesolvents used for the processes and the conditions.

Chemical absorption is a mature technique which is commercialized for a longtime to remove CO2, but it has serious disadvantages which keep them on hold.

Alkanolamines are the commonly used solvents for CO2 capture, and the reac-tivity varies based on the primary, secondary, or tertiary nature of the amine with atleast one hydroxyl group. The reactivity of CO2 with the amines will be in the orderof primary >secondary > tertiary, which is understood based on the reactionconstant of values of 7000, 1200, and 3.5m3/s/kmol for MEA, Di ethanol amine(DEA) and N-methylethanol amine (MDEA), respectively, at 25C [112–114].Whereas the loading capacity of these amines is exactly opposite, primary amineand secondary amine have a loading capacity of 0.5–1 mole/mole of amine and aloading capacity of 1 for tertiary amine. For a schematic representation of primaryand secondary amine reacting with CO2 in presence of water and formation ofbicarbonates, see Fig. 5. The reason for the difference is the tertiary amines formbicarbonates with CO2 where the ratio is 1:1, whereas in the case of primary andsecondary amine, first the amine forms a zwitterion with one mole of amine followedby conversion of this zwitterion to carbamate in presence of another mole of amine[115–117] (1:2).

Mixed amines were preferred over single amine compounds in order to increasethe efficiency of CO2 capture (see Fig. 6.). The efficiency is still increased when theused amines are sterically hindered, as the steric hindrance makes the carbamateunstable and undergoes hydrolysis to form bicarbonate. This reaction releases theamine back which will be reused; thereby the efficiency was maintained to 1:1 mole/moleCO2 similar to tertiary amines. Sterically hindered amines, for example, 2-amino-2-methyl-proponal (AMP) [118–122], were found to have higher selectivityand efficiency. Cyclic amines like piperazine were found to improve the efficiencystill further as they are used as a promoter to capture CO2 because of its rapidreaction with CO2 to form carbamate [123, 124]. Piperazine (Pz) resists degradationat high temperatures, but its limited solubility in water requires a high amount of Pzto carry out efficient CO2 capturing.

The main issue with the alkanolamine is their stability. They undergo three typesof degradation which increase the operational cost and possess environmentalproblems. Degradation can be induced by heat or by dissolved oxygen or carbamatepolymerisation [125]. The amines start degrading generally above 200 �C which


limits their usage from regeneration point of view. Oxidative degradation due todissolved oxygen happens when the dissolved oxygen content was above 5% [126,127]. Carbamate polymerization happens at high temperature in the stripper duringthermal regeneration [128]. This amine stripping process was found to an energyintensive process as it consumes around 60% of its energy for the regenerativepurpose, which increases the overall cost of the process [129].

Apart from being used as such, it can be used in combination with other amineslike MEA, diethylene triamine (DETA), and AMP to increase the efficiency in theform of blends of different ratio [130–137]. As per simulation studies by Dash et al.[138], it was proposed that a blend of AMP and PZ with a wt% of 22 and 8 will givea CO2 absorption efficiency of 90%.

Table 2 Commercialized industrial process for removal of CO2 by using solvent adsorptionprocess and their efficiency [111]

Process Solvents/chemicals Conditions Advantages

CO2

solubility@ 25 �C(ft3/US gal

Selexol Dimethylether ofpropylene glycol(DEPG)

Can remove bothCO2 and H2S[110]

Can be operated at lowvapor pressure, lesstoxic, less corrosive tometals

0.485

Rectisol Methanol For flu gascontaining sulfurfrom refineries

Less corrosive andmore stable absorbent.Operates at lowtemperature

0.425

Purisol N-Methylpyrolidone(NMP)

Suited forpurification ofhigh pressure,high CO2

Synthesis gas

Consumes less energy.Operated at ambienttemperature or temp upto 5 �C

0.477

Fluor Propylene carbonate(PC)

More suitable forCO2 partialpressure higherthan 60psig

Solubility of CO2 isvery high

0.455

RNH

CO2

R'

RNH

R'

O

O

RNH

R' RN

R'

O

O

RNH2

R'CarbamateZwitter ion

H2O

RNH2

R'HCO3

-

Fig. 5 Schematicrepresentation of primary andsecondary amine reacting withCO2 in presence of water andformation of bicarbonates


Other absorbents like aqueous ammonia with the additional absorption of SO2,NO2, and value added product formed after reacting with CO2 for fertilizer industryhave high efficiency with low energy recovery cost [139–151]. This absorber wasupgraded to pilot scale because of its distinct advantages [147].

Another absorbent which has got the potential to be used for industrial applica-tions is aqueous K2CO3. It has got all the credentials required for an absorbent excepthigh mass transfer rate [148–158]. This is overcome by adding inorganic and organicpromoters like salts of Ar, V, B, and amine and their derivatives, alkaline amino acidslike arginine and even biological enzymes like carbonic anhydrase. For example, theefficiency of K2CO3 with MgO was fed to show an efficiency of 99.4% for CO2

[159].Due to the enormous advantages of ionic liquids, they were also exploited

towards CO2 capture. ILs capture CO2 via both physical and chemical absorption.Physical absorption in IL happens based on the size, the ions (anion and cation), andfree volume. The CO2 solubility mostly depends on the anions and does not have anyeffect on cations used in IL [160]. The CO2 solubility in bis(trifluoromethylsulfonyl)imide (Tf2N) was higher than those in tetrafluoroborate (BF4) and hexa-fluorophosphate (PF6), indicating the more significant effect of anion onCO2 solu-bility. ILs for chemical absorption proceed in presence of amine functionalized ions,

H2N

H2N

HN

NH2

OH HOHN

OH

HON

OH

HO

HO OHH2N *

HN

*n

NH2SiO

OO

Monoethanolamine

Diethylenetriamine

Diethanolamine

Triethanolamine

2-amino, 2-methyl, 1,3-propanediol Polyethyleneimine (PEI)

3-aminoproplytriethoxysilane (APTES)

HNNH

Piperazine

Fig. 6 Structure of representative liquid sorbents for capturing CO2


which reacts with the CO2 and the adsorption capacity was drastically increased 3–4times compared to physical absorption [161]. The limitation with this aminefunctionalized ILs is their viscosity which arises due to the formation of hydrogenbonds between anion and cation. Viscosity, as well as the absorption capacity ofCO2, can be increased by using supported IL. The CO2 capture capacity for[aP4443][AA] was just 0.2 moles of CO2 per mol of IL as viscosity restricts furtherabsorption. The same material when supported over silica gel the absorption capac-ity was increased to 1.2moles of CO2 per mol of IL [162]. The porous surface withthe high surface area also gets involved in physical absorption which increases theoverall efficiency of CO2 scrubbing. The viscosity and absorption capacity isincreased when the ILs are blended with alkanolamines [163, 164]. Functiona-lization and immobilization of PEI over solid adsorbents like silica or other carbo-naceous material were the recent approaches to curb the atmospheric CO2.

In the case of water lean solvents [165], the CO2 capture involves two distinctsteps one is solvation and other is binding. First, the gas gets solubilized into theorganic solvent and followed by chemical binding to form either alkyl carbonates orcarbamates or azoline carboxylates and other acid/base reactions like proton transferor dehydration. The nature of binding in these systems should be of low energetics inorder to be regenerated for further use.

Usage of amine-based solvents in presence and absence of water has bothadvantage and disadvantage. In presence of water, the regeneration temperaturewill be high compared to organic solvents. So a blend of organic solvents withaqueous amine sorbents was found to be much better than the pure amine sorbents.Some examples are N-MDEA in methanol [166], TEA in alcohols [167], anddiethanolamine in ethyleneglycol [168]. These solvents were used in conditionswhere the high-pressure flue gas is available. These co-solvents were found toincrease the solubility of CO2 and the adsorption capacity which is advantageswhen compared to the usage of volatile organic solvent in industrial scale which isimpractical and cost effective. Nonaqueous organic solvents derived from amineswere also used [169–172], such as 2[(1,1-dimethylethyl)amino]ethanol and 1-[(1,1-dimethylethyl)amino]-2-propanol. The amines reversibly bind CO2 to form carbon-ate zwitterion (See Fig. 7), which will be regenerated at a lower temperature than theaqueous amine solvents. The zwitterion carbonate formed mostly will be solid innature and can be easily removed and purified [169].

Similar to these two solvents, other nonaqueous organic solvents derived fromamino silicones [173–175] and switchable carbamates [176] are also designed topromote the adsorption capacity. Other types of solvents that are used are:

(a) Super base promoters [177], where primary amines combined with the strongnonnucleophilic base as a secondary component have been seen to show anenhanced CO2 capture

(b) Amino acids in organic solvents [178–180](c) Alkylcarbonates [181–184](d) Heterocyclic azoles [185–187](e) Hybrid systems with nanoparticles [188–190]


AdsorptionAnother process, which can be exploited more for CO2 sequestration is adsorption.Though both physical and chemical absorption process have some economicaladvantage in the form of cheap commercially available raw materials, they havesome series drawback, which makes the scientific community to look into otherpossibilities. The main problem in the case of liquid sorbents is the low mass transferat the gas-liquid interface, because of this CO2 adsorption capacity will decrease. Ifthe sorbent is having any other dissolved gases (O2), that too will reduce theadsorption capacity. Presence of dissolved oxygen in presence of the sorbent willalso induce absorbent corrosion [191] which will damage the equipments perma-nently. Adsorption of gas over the solid adsorbents will be a viable and economicalprocess because the area exposed to surface adsorption is much higher than theliquid absorbents. Another interesting factor which makes adsorption superior overabsorption is their rate determining steps. For adsorption, the rate determining step isthrough a gas diffusion process inside the pores of mesoporous adsorbents, which is3 times in magnitude higher than the absorption process whose rate determining stepis mass transfer [192].

Numerous solid adsorbents have been proposed considering different structures,compositions, adsorption mechanism, and easy regeneration. All these adsorbentshave to qualify certain criteria in order to be used as an efficient CO2 adsorbentmaterial. Some of them are (a) low-cost raw materials, (b) low heat capacity, (c) fastadsorption kinetics, (d) high CO2 adsorption capacity, (e) selectivity towards CO2,and (f) thermal, chemical, and mechanical stabilities in order to be recycled effi-ciently without loss in any of the above said properties.

Carbonaceous MaterialsCarbon-based adsorbents are of interest and promising, as they can be derived frombiomass, due to their high surface area, due to the high possibility of functiona-lization and along with that due to high porosity. These properties make thesecarbonaceous materials amenable for gas sorption [193] especially CO2.

Functionalization over the carbonaceous materials can be done in many ways toimprove the adsorption; some are microwave irradiation, impregnation of metals,

RNH

OH CO2 RNH

O OH

O

RNH2

O O

O

Alkanolamine Carbamate

bicarbonate

Fig. 7 Schematicrepresentation ofalkanolamines reacting withCO2 to form zwitterioncarbonate


modification with the base, impregnation with amine solution, and many more[194–196]. Microwave treatment decreases the amount of surface oxygen on thematerial and increases the surface area and porosity. Apart from this, the processbrings in basic characteristic to the surface, which increases the attraction of acidicCO2 group. Zhang et al. modified AC in presence of N2 under microwave irradiationwhich increased the surface area to 2546 m2/g with sorption capacity of CO2 to3.75 mmol/g.

Some of the biomass-derived carbonaceous material for activation towards CO2

capture are palm oil shells [197, 198], olive stones [199], almond shells, coconutfibre [200], used coffee ground [201], bamboo, etc. All these biomass-derivedmaterials are functionalized or modified in order to be used as a better sorbent forCO2 abstraction from the atmosphere, and the preliminary results were very prom-ising which shows their potential for scaling up in industries [202].

Greener adsorbent like porous silica sand and silica gel was used in combinationwith clathrate hydrate process and the former was found to perform better than thelatter [203]. These adsorbents apart from being greener have high selectivity, easyregeneration, high stability, and more important cost effective in nature. Othergreener products like olive stones and almond shells are used as carbon adsorbentswith high adsorption capacity of 48 mmol/g at 101kpa at 0C [204]. Macadamia nutshell-based carbon composites showed an efficiency of 35% in postcombustionprocess [205]. Bio char from sugarcane bagasse, hickory wood, and eucalyptuswood-based activated carbon modified by ammonia adsorbed at 73.55 mg/g at600 �C was reported by Gao et al. and Yonnesi et al. [206, 207]. To increase theselectivity of CO2 in a mixture of nitrogen, methane, carbon monoxide, and oxygen,porous synthetic hectorites (clay type minerals made from LiF, MgO, SiO2) wereemployed which showed an adsorption capacity of 22.8cm3/g and 18.7cm3/g withand without modifiers, respectively [208].

Compared to liquid-based adsorbents, solid adsorbents with varying structures(micro, meso, and nano) have the highest potential towards CO2 capture and forcommercialization. Another commonly used type of adsorbent called zeolite withvarying SiO2/Al2O3 when modified with PEI improved the efficiency 24 timeshigher than the neat zeolite (MCM-410, but it cannot be used in postcombustionindustrial process as its efficiency was low and not attractive.

An additional increase in the efficiency will be achieved if the oxide surfaces arefunctionalized with more basic groups like amines. These amines can either begrafted over or just dispersed, with higher the incorporation, better the efficiency.Different amines were utilized among those, and PEI and amino silanes were foundto be highly efficient. For example, around 60 wt% PEI impregnated HMS zeoliteswere found to adsorb around 184 mg/g CO2. In another case, the efficiency increasedup to 7 times for tri-ethanol amine impregnated SBA15 when compared to neatSBA15. It is also found out that presence of OH functionalization will increase theefficiency. So a mixture of amine and hydroxyl groups on the surface will yield CO2

sequestration efficiency more than just NH2 or OH or oxide surface. The presence ofOH groups will increase the probability of reactive amine sites by half whencompared to just amine modification. This will also increase the saturation capacity


of the material by twice which is clearly understood by the stoichiometry of theabove equations.

Activated carbon is the another type of adsorbents proposed for CO2 due to itslow cost, high thermal stability, high resistivity to moisture, and wide availability[209], but by performance, wise activated carbon cannot be used where the flue gaspressure is low. To improve the adsorption capacity, the carbonaceous materials arefabricated using different precursors to form ordered mesoporous structures withhigh surface coverage (Zeolites), like Single wall CNT, Multi walled CNT, Graphene[210, 211], etc. Adsorption can also be improved by modifying the solid adsorbentsurfaces which can increase the alkalinity, whereby the acidic CO2 can adsorb veryefficiently. Zeolites efficiency towards CO2 capture is affected by the size of thepore, charge density and chemical composition of the basic group. Some modifica-tions toward improving the efficiency are altering the Si/Al ratio, substituting alkaliand alkaline earth metal cations. Mesoporous silica with high surface area, high porevolume, tunable pore size, and good thermal and mechanical stability makes thesematerials an interesting candidate for CO2 adsorption. Some of the most famousmaterials used for this cause are M41S, SBA-n, anionic template mesoporous silica(AMS) [212–214], etc. These materials are not efficient enough to adsorb CO2 for itsfull capacity especially at atmospheric pressure, which limits their practicalapplication.

Adsorption technique has the advantage of easy desorption of CO2 and regener-ation of the reactive material. For this, many porous materials were designed andused extensively. Each one has its own limitation and modern research has sophis-ticated tools in inventing novel materials which provide a wide range of porosity.Some of the porous materials are zeolite based molecular sieves, activated carbons,carbon nanotube (CNT), graphene, etc. The order of efficiency stays in the sameorder where activated carbon (AC) is better than zeolite, and CNT is better than AC.Due to higher surface area and high porosity. Graphene having the tetrahedral framein 2D form has the better adsorption capacity than other due to higher SA than CNTs[215–220].

CNT finds wide application in modern era [221]; one among them is to utilize itsefficiency in gas adsorption and storage. Instrumental studies suggest gas adsorptionis a viable process for purification but some specific conditions complicate theseparation process as theoretical conditions are not 100% possible in industry[222]. Despite these difficulties, one work was done on CO2 capturing over grapheneat experimental conditions for practical application in CCS technology.

Hydrogen exfoliated graphene (HEG) was found to have a large hysteric area fornitrogen adsorption-desorption isotherm from BET analysis [223]. Adsorption iso-therm for CO2 at 3 different temperatures (25, 50 and 100 �C) and 11 bar pressurewas found to show a decreasing trend with values of 21.6, 18 and 12 mmol/g,respectively. The decrease in efficiency with increase in temperature might be due tothe increased kinetic energy which increases the possibility of desorption. Withdecreasing pressure, the desorption capacity is high, which is highly encouragingto remove the CO2 and utilize the matrix for further use. The main disadvantage ofthis process is that the pressure of the inlet gas has to be maintained very high and the


concentration should be high enough to have maximum adsorption. Playing with thepressure and temperature will lead to an optimum condition which will be exploitedfor CCS. A comparative study on graphene oxide (GO) for CO2 adsorption withactivated carbon and zeolites shows that HEG was found to be much superior andhas the proximity to be implemented for large-scale CCS [224].

Some of the adsorbents which can be used at higher temperature are calciumchabazite, 13þ zeolites, and K2CO3-based HTC zeolite, hydrotalcite (clay minerals)with embedded nickel and iron cations with and without boehmite alumina. Thesecompounds were found to be very stable at high temperature with a maximumadsorption capacity of 2.5 mmol/g [225]. Among the amine- and carbon-basedadsorbents, amine-based sorbents exhibit high adsorption capacity, whereas thecarbon-based material showed stability for recyclability, even though the capturingefficiency is low [226]. Some of the carbonaceous materials with Nano porousstructure with a size of 1–100 nm are zeolites, activated carbon, nano too structuredmaterial (1–10 nm) like carbon nanotubes, CaO nano pods, nano crystalline particleslike lithium silicate, Li2ZrO3, etc. Apart from these synthetic materials, naturallyexisting materials and industrial wastes like slags, fly ash, filler cakes, foundry sands,dusty from the cyclone, furnace, and cement kiln are employed for CC [227, 228].Among these fly ash is a potential candidate for CC [229].

PEI modified mesoporous carbonaceous material with a % loading of 65% wasfound to show a capacity of 4.82 mmol CO2/g sorbent [230]. KOH activated pitch-based mesoporous carbonaceous material showed a potential of 203 mg/g towardsCC technology. Hetero atom functionalized carbon-based materials show a sorptionof 8 mmol/g for N functionalization and 3.21 mmol/g for S functionalization whichare activated by KOH [231, 232].

Chemical Adsorption Using AminesFor chemical adsorption, the adsorbing group has to form a covalent bond, which ispossible only when the acidic CO2 groups react with a basic group on the surface ofthe solid adsorbent. The basicity over the solid surface can be brought by impreg-nating or functionalizing with organic amino groups or highly basic metal oxides(alkali and alkaline earth materials). Amine content over the surface can be incor-porated by two ways: by amine grafting and the other by amine impregnationthrough weak interaction and strong covalent bonds [233]. Comparatively, aminegrafted adsorbents have higher adsorption capacity and high stability for cyclic runs.But the limited amine groups grafted over the sorbent due to less available surfacesilanol groups which control their efficiency.

Metal OxidesMetal oxides with different structures were turning out to be one of the potentialmaterials for CO2 sequestration. The reason for that is that these metal oxides canretain their structures irrespective of their size (macro, micro, or nano). Because ofthis, the efficiency will also be improved due to surface area. Another critical pointwhich makes these metal oxides unique is their reactivity to CO2 to form thermo-dynamically stable carbonates. The formed carbonates can be easily converted to


CO2 and respective oxide by simply heating. The carbonation reaction between thegas and oxide was exothermic, the decarbonization reaction was endothermic, andthis forms the cyclic process, but specific pressure and atmospheric conditions haveto be maintained to achieve better efficiency in both the processes. With respect tothe metal oxides, there are more scopes and pot holes in utilizing the metal oxides totheir fullest. Depending on their availability in nature, different MOs have differentinherent properties like durability, mechanical strength, etc. The adsorption capacityof MOs has to be analyzed before using it for CO2 sequestration process. Availabil-ity, cost, regeneration temperature, kinetics, recyclability, and durability should beconsidered before selecting any metal oxide for a large-scale application [234–237].

The flue gas conditions vary depending on the way it was burnt; for pre-combustion conditions (where the stream has CO2, water, and hydrogen), thepressure of CO2 will be between 20 and 25 bar and the temperature will be300–350 �C. The partial pressure of the same gas at postcombustion conditions(gas stream has CO2 and N2) will be between 0.1 and 0.2 bar and the temperaturewill be between 27 and 77 �C [238]. This varying condition brings in the need toselect the oxide which can give better adsorption and desorption at lower energyconsumption. Some of the oxides and mixed metal oxides, which were found to bepromising in the field of CO2 sequestration, are CaO, MgO, Li, Na, FeO, and Ksilicates. The rate determining step for sequestration of the gas using metal oxide isits diffusion across the interface to undergo a reaction, which will form the carbon-ates or bicarbonates or other products. To improve the diffusion, either temperature[239, 240] is varied or the structure modified with dopants or the surface areamodified or the structural arrangements should be varied. Metal oxides dopants,for example, K2O3 and Y2O3 to Li2ZrO3, were found to increase the CO2 sorptionkinetics. In the case of pure Li2ZrO3, typically the oxide forms a coating of Li2CO3

over the oxide, thereby inhibiting further reaction of CO2 with the core. In the case ofmixed oxides, the dopant forms a eutectic mixture, which at high temperature allowsthe CO2 to diffuse into the shell [241].

Lithium silicates were interesting oxides for CO2 sequestration, though theworking temperature is high from 250 to 550 �C at 0.2 atmp. An interesting fact inall these oxides is that the CO2 adsorption rate increases or gets altered in presence ofmoisture. Lithium silicates are effective in separating H2S from the feed stream apartfrom the CO2. Oxides based on sodium were found to be economical than its counterparts like K, Li, etc. Even their efficiency is better, for example, compared toLi2ZrO3 and Li4SiO4, Na2ZrO3 is highly reactive [242]. Here too the mechanismis similar to the one explained earlier, which is based on the diffusion of the gas andthe metal oxide. The reaction will be as follows:

Na2ZrO2 þ CO2 ! Na2Co3 þ ZrO2

As mentioned earlier the reactivity will change in presence of moisture. So, thesame oxide in presence of water tends to form bicarbonates instead of carbonates[243, 244].


Na2ZrO2 þ H2O ! Na2ZrO3

superficiallyhydrated

þZrO2 !CO22NaHCO3

Nano-sized materials will increase the CO2 capture and regeneration due to theirhigh surface area and high surface reactivity. The interaction or the reaction depictedabove all happens due to the presence of unsaturated bonds or other functionalgroups on the metal oxide surface [245–247].

The crystalline structures also influence the CO2 capture, for example, formonoclinic Na2ZrO3, the CO2 capture was more than the hexagonal structuredNa2ZrO3 [248]. Lithium content also has an influence; with increasing lithiumCO2 adsorption decreases and with increasing Na content the adsorption decreasesbut material properties increased [249].

Metal Oxide Framework (MOF)Separation of greenhouse gas at high and low partial pressures from the point of thesource has been addressed by the scientist with a wide variety of options andattractive solutions. One among those is sorbents-based polymer matrixes with thewide option of polymers and sorbents. The sorbents can be both of organic andinorganic in nature [250]. Inorganic sorbents will be mostly oxides of alkali andalkaline earth metals; one step ahead of these oxides, oxides with ordered structurescalled metal organic frameworks is the recent sorbent which was tuned to adsorbmore amounts of CO2. Work on these type of mixed matrix membranes (MMM)formed by dispersing inorganic or carbon-based sorbents such as nanotubes in apolymer blend will increase the diffusion or permeability of the gas along withselectiveness [251–264].

MOFs are of the recent materials which have attracted interest for CO2 adsorp-tion. These materials have the remarkable high surface area, uniform pore sizes, andtunable pore surface properties by just changing the metallic clusters or the organicligands used to make the MOFs. MOF with cavities has high CO2 capture potential,low energy consumption for desorption, and higher impurity tolerance. The surfacearea for MOF will be in the range of 1500–4500 m2/g which is very high comparedto the surface area of 400–1000 m2/g of activated carbon and 1500m2/g of zeolites.MOFs for CO2 capture was first reported by Yaghi’s group [265], following himmany groups started working on MOF’s for CO2 capture [266–269]. The resultswere much promising under lab scale with MOFs, but it requires a number ofresearches to convert these lab scale projects to industrial scale.

Recently amine modified TiO2 nanotubes, TEPA-modified metal organic frame-works (Mg-MOF-74) showed the highest adsorption efficiency of 167.64 mg/g withgood cyclic stability [270–272]. PEI modified MOF was found to have an increasingselectivity towards CO2 over Nitrogen with temperature with a value of 770 at 25 �Cand 1200 at 50 �C [273]. The adsorption capacity of this material with a flue gas at15 wt% of CO2 and 400 ppm was found to be 181 mg/g and 99.3 mg/g at 25 �C,respectively [274].


Flexible MOFs are additional boon to CO2 sequestration process because thestructure can be squeezed or expanded depending on the amount of adsorption; thisflexibility gives a unique result for the adsorption-desorption process. These mate-rials have unique adsorption isotherms, where there is a rapid adsorption after athreshold pressure and a hysteresis desorption isotherms, which is possible byopening up of the pore structure above a critical activity or threshold pressure[275–280]. Zornoza et al. demonstrated this behavior by incorporating flexibleMOFs in a MMM, which showed an increasing CO2/methane selectivity withincreasing pressure [281]. A similar kind of work was done using Ni(Bpy)(DBM)2MOF with different polymer structures like Matrimid, PS, and polysulfone. Theseflexible MOFs are host specific and the results were found to be interesting when thehost is CO2, which changes the structural phase which was proved by adsorptionisotherm and in situ ATR-FTIR spectroscopy. But the results were not in line withthe earlier work by Zornoza, which might be due to the difference in the degree ofswelling during the CO2 adsorption process. These contrary results, when provedwith substantial data, will be a unique technique for the CO2 sequestration process,which further needs extensive research to come to a conclusion [282].

Pressure swing adsorption and temperature swing adsorption are some of thetechniques for CO2 removal from the gas stream. Pressure, temperature, and elec-trical swings have been employed for effective adsorption-desorption process drivenby physical or chemical sorption. All these properties are directly related to theirpolarity, surface area, pore size, and spacing of the selected adsorbent.

Membrane TechnologyA technique which can be commissioned at comparatively low cost, which can beused continuously with very low start up times and at high product purity, can beachieved by using membrane technology. Membranes can be designed to separateCO2 from flue gas mixture as different gases have different diffusivity or perme-ability [283–285] which gives the selectiveness for the separation or purification.Inorganic membranes can be synthesized using ceramics, zeolites, metallic, etc.,organic membranes can be designed by crosslinking organic polymers with knowncrosslinking density and predetermined permeability. The disadvantage of thistechnique will be its work function at low CO2 concentration, high flue gas temper-ature, and the possibility of fouling restricts their application for their self-life.Membranes with novel functionalities or using different compatible blends or withbiomimetic configuration are the novel areas for making membranes for future workand application [286–288].

In membrane technology, an effective membrane system for CC has to beendorsed with high adsorption capacity without CO2 penetration into the bulk,high recyclability, highly selective to CO2 with insignificant sorption capacity toN2, CH4, H2, and others in flue gas, high resistance to flue gas, resistance topoisoning by SOx, NOx, and H2S, ease of fabrication, high stability at elevatedtemperature and ability to perform efficiently at lower thickness [289]. Membranetechnology can be used for both pre- and postcombustion process for CC technol-ogy. The membrane system is developing into a process intensification tool for


reactive adsorption processes. It is reported that around 35% cost reduction can beachieved by this membrane technology.

Membranes can be designed using polymers or using an inorganic material withporous to non-porous structures. These membranes act as a filter and selectivelyallow one gas to permeate. Advantages of membrane technology over other are thatthere is no overflowing of penetrant or unloading at the low flow rates, high surfacearea per unit contact volume, independent control of gas, decreased flow rate,compactness, and scalability [290].

All these advantages overweigh the fouling problem due to membrane composi-tion [291]. They offer low maintenance cost, relatively low capital cost, and smallphysical foot print which makes it favorable for less energy intensive operations. Themain issue in the form of designing a membrane is to have a uniform porosity andthickness, with nonwetting characteristics, hydrophobicity, nonpolar nature, andpore size distribution. The other factor which will influence the separation processwill be the flue gas composition, operational temperature, and flow rate, etc. [292].Different types of membranes were designed depending on the usage andparameters.

Microporous MembraneInorganic membranes and facilitated transport membranes fall under this category.PVDF (polyvinylidene fluoride) PP, PTFE, PEI (polyetherimide), PSf (polysulfone),PMP (polymethyl pentene), and Teflon-AF are some of the membrane materialswhich can form mesoporous structures [293]. PP is economically cheap but withvery less chemical resistant, whereas PVDF and PTFE are costly but good inchemical stability. The gas passing through the membrane gets adsorbed inside thematrix pores, whose performance can be improved by crosslinking with aromaticgroups as hyper branches. Recent hyper branched linkers in the polymer chain canimprove the porosity and it has the additional benefit of surface functionalities [294].Microporous membranes with amine functionalization were also designed for CO2

adsorption in CC process, which was found to be efficient [295]. More research hasto be done to have better membranes with high stability and better selectivity to beused commercially with less fouling.

Dense MembranesThese types of membranes were used successfully for CC process which shows ahigh permeability and flux [296]. Tf2N, ceramic, ceramic composites, PDMS, DMS,PSf, pebax, polyamide-imide, PPO, PVAm, CNT, LDPE, PEEK, PBD, polyure-thane, and still more were used as the starting material for membrane formation[297]. PEG-based MWCNT and Pebax blended membranes [298] were found toshow high CC efficiency with selectivity of >100 and permeability of 743 barrier(1 barrer= 7.5� 10�11 cm3(STP) cm/cm2skPa). Stability towards high pressure wasobtained by designing a mixed matrix membrane of PVA containing amines withMWCNT [299]. A novel hybrid membrane system made using K2CO3-dopedanhydrotalacite catalyst was used for precombustion CC process and hydrogenproduction [300, 301].


Supported Liquid MembranesThis technology is a novel methodology for CC process, which showed promisingresults in the lab scale experiments and is ready to be up scaled for commercialpurposes in industries [302, 303]. Here the principle is the reactive liquid is dispersedover a porous or nonporous support. The flue gas or the gas which has to be treatedeither undergoes chemical or physical adsorption into the liquid, where the liquidplays an important role in the mass transfer process. Ionic liquids supported overzeolites or polymers were the common examples. DEA supported on PVA, ionicliquids [hmim][Tf2N], [emim][CF3SO3], [omim][PF6], enzyme of carbonicanhydrase, etc [304]. Ionic liquids eliminate the purification stage or solvent evap-oration step for recovering the support or the gas in the CC process, which willreduce the cost of the overall process [305].

Cryogenic Process

Another technique which is gaining attention under CCS process is cryogenicseparation. The advantage of this process is that no chemical absorbent is neededfor the success of this process [306–308], and it can be used at normal atmosphericpressure which makes them easy to transport in the liquid form along with othercompatible mixtures. But this process has some disadvantages, such as the formationof CO2 clathrates with water molecules, which brings plugging issues, pressure build-ups, and reduction of heat transfer rates due to thick CO2 layers formed on heatexchange surfaces. Purification of atmospheric air using cryogenic distillation to getpure oxygen for combustion is an age old process which has been practiced over100 years [309]. Typically the air is compressed to a pressure of 0.5–0.6 MPa wherethe impurities like water, carbon dioxide, nitrous oxide, and trace amounts ofhydrocarbons will be removed. The impurities will be adsorbed and regenerated bytemperature or pressure swing and can be sequestered. The pure oxygen stream willbe fed for power generation. Some of the noted processes for cryogenic separation areRyan Holmes method [310], the controlled freeze zonemethod [311, 312], the cryo-cellmethod [313], twister technology [314], and the sprexmethod [315]. The separa-tion by the cryogen occurs due to a decrease in the internal energy of the CO2 [316].

Chemical looping combustionChemical looping combustion (CLC) is the advanced technique of OFC which usesmetal oxides as the source or fuel for combustion. This is an inherent CC process dueto the formation of CO2 and water as products with minimal formation of NOx gases[317–319]. This process is still in the lab scale which will take more time to getcommercialized. Chemical looping combustion (CLC): It is a postcombustion pro-cess, which is a promising clean technology developed for CC, which minimizes thedilution of CO2 with flue gases. Principle [320, 321] behind CLC is splitting thecombustion of fuel into separate oxidation and reduction process by using metaloxides as the oxygen carrier which will be cycled between the two process kept intow chambers. A schematic representation is given in Fig. 8. The process for


purification of atmospheric air to get pure oxygen for combustion is omitted as theoxygen will be fixed by the metal as metal oxide (Oxidation). The oxidized metal issent to another chamber with fuel where the metal oxide gets reduced by releasingthe oxygen for combustion with the added fuel to give the heat, and in the process,the pure metal is recovered and ready for another cycle. Compared to the conven-tional single stage combustion, the two stage process in CLC is much superiorbecause the CO2 produced by the above redox process is not diluted with nitrogenwhich reduces the extra energy to purify the outgas stream. Some of the metal oxidesused for this purpose are from common transition metals like iron, copper, nickel,and manganese [322]. The size of the metal/metal oxide is more important as it has tobe fed to the chamber easily. The optimum size should be in the range of 100-500micrometer. The temperature in this process will be in the range of 800-1200C. Itis estimated that the efficiency of natural gas fuel to electricity will be in the range of45–50%using CLC process.

Sequestration of Captured CO2

Sequestration of the pure CO2 stream at a well-managed geographical storage site isbeing considered as a mitigation option for climate change. But the cost factorinherited (including transport, compression of the gas, find the respective well, itscapacity, etc.) with those processes is high, which reduces their widespread instal-lation. However, it is widely accepted that there is a large scope for cost reductionand energy efficiency improvements in CO2 capture systems.

Geological Sequestration of Carbon Dioxide

The CO2 separated from the BECCS, DACS, and CCS process has to be concen-trated and sequestered to prevent its return to the atmosphere. Some of the ideal

Fig. 8 Representation of chemical looping combustion process under oxy-fuel combustion


geological sites or places for sequestering the gas are depleted hydrocarbon reser-voirs, coal beds, and saline aquifers. The capacity of these sites varies with anestimate of ~1000GtCO2 from depleted oil and gas reservoirs, 200GtCO2 for coalbeds and a variable data of 4000 to 23000GTCO2 for aquifers [323]. Presently thereare over a hundred selected sites all over the world for injecting CO2 undergroundeither as storage site or for enhanced oil recovery or to prevent toxic acid gases beingreleased to the atmosphere by mixing with H2S.

Injecting the gas under the reservoirs for EOR will lead to the additional recoveryof hydrocarbons which will be the source for another cycle of CO2 in the atmo-sphere. But this process generates revenue and also the dying reservoir can be givenlife for some more years. Deep saline aquifers are distributed very scarcely and theyare generally used to dispose of anthropogenic CO2. For example, India and Chinahave a significant number of coal fired power generation plants but not oil and gasreservoirs and there comes the usage of the saline aquifer storage in these regions,whereas in USA and UK they have a huge number of oil and gas reservoirs [324].The following are some of the parameters which have to be known before using thestorage sites for sequestration.

Storage capacityBefore the gas is injected into any wells, an approximate capacity of the well has tobe estimated which is easy in the case of oil wells, where we get an estimate of the oiltaken out, but in the case of saline aquifers, it is not that easy to calculate. Theseestimates are a normally simple fraction of estimated pore volume. But the actualamount depends on the number of wells drilled, what sort of wells and whether ornot brine is produced.

Storage mechanismThe gas is injected by converting it into supercritical liquid, which weighs as liquidand flows as gas. This supercritical fluid under lower pressure conditions starts toexpand and changes its phase to gaseous phase. There are different principles bywhich the injected gas is prevented to reach the surface: one is cap rock, other onedissolution, reaction, and capillary trapping.

Rocks which have low permeability are called as cap rocks. These low permeablerocks act as a capper to avoid the gas to diffuse upward which is similar to trappingoil. These rocks are made of salt or shale or clays with very small pore size than theCO2, which prevents the gas to permeate as the pressure underneath is not sufficientto enter.

Dissolution of the gas in brine will keep the gas under the sink as it will form adenser phase. The solubility of gas will be high at high pressure in water, whereas thesolubility decreases in more saline condition. For example, 6% NaCl solution willdissolve approximately 30–40 kg/m3 of CO2 at a temperature of 80C which repre-sents a reservoir condition at 1000 m, where the temperature rises due to the earth’score.

The dissolved gas reacts with the brine solution to form carbonic acid which is aweak acid and reacts with the rocks to form the carbonates. This process takes over


thousands to millions of years under the sub terrain conditions, thereby trapping thegas inside over these many years. This is a complex geochemical process, where theoxides of the rock dissolve and precipitate as carbonate.

This happens when the water displaces CO2 in the pore space. Fig. 9 shows thetrapped water under the rock in pores. The CO2 inside the pores of the rock getstrapped or surrounded by the water well, thereby inhibiting the gas to escape [325].

DrawbacksSome of the negative aspects of geological sequestration are leakage, the risk ofinducing seismic event through over pressurizing the reservoir, long-term integrityof cap rocks, etc. A recent study by Gan and Frohlich [326] suggests that injection ofthe super critical CO2 since 2004 in Cogdell oil field north of Snyder, Texas, mightbe the contributing factor to seismic activity happened between 2006 and 2011 witha total of 18 earthquakes of magnitude >3.

The same injection activity might affect the seal integrity and might increase thepotential for leakage. The leakage density varies with time, where it decreases due tosecondary trapping mechanism like getting dissolved in saline water. The high densesalt water containing CO2 will automatically sink to the bottom of the ocean bed andgets trapped. Another option is mineral trapping where the gas gets converted tocarbonic acid which reacts with the minerals in the rocks to form carbonate mineralsand gets permanently trapped. The risk associated with the transport of CO2 throughpipelines will be chocking and leakage due to accidental damage. Since the gas ismuch denser, it stays at the ground level leading to respiratory risks (Asphyxia) athigh concentrations.

Value Added Application of CO2

The primary market for CO2 is EOR; apart from that food beverage industry,chemical markets also use CO2 but to a lesser extent. In the USA, about 54MtCO2

was used for EOR and most of them are sourced naturally (80%) rather thananthropogenically. About 80-120Mt CO2 was sold commercially for the chemicalindustry as a solvent, for coffee decaffeination, fertilizer production and carbonated

Fig. 9 Trapped water underthe rock in pores


beverages, 1MtCO2/year for refrigerants and solvent, and ~8MtCO2/year for thebeverage industry. Sridhar and Hill (2011) have estimated a reduction of 1.6Gt/yearof CO2 when the regular composite material for buildings is replaced by carbonateminerals-based composites [327].

Conversion of CO2 to value added products [328] is one of the safest ways toutilize the dangerous gas with nil or negligible side effects which is a great advance-ment in the journey for low carbon footprint. Recently scientists from Paris DiderotUniversity, France, and National university of Cordoba, Argentina, have developed acatalyst which will convert Atmospheric CO2 to methane using visible solar light asthe catalyst. The research is in its infancy, which will be developed to a pilot scalelevel. The researchers illuminated CO2 saturated solution of ACN containing anelectron donor, a photosensitizer, and a small amount of iron phenylporphyrincatalyst functionalized with trimethylammonia groups. The whole process is eco-nomical as the raw material and methods to make the catalyst are very less. Themajor and interesting result from this group is that the selectivity of convertingaround 82% of CO2 to methane. The initially reduced CO from CO2 furtherundergoes catalytic reaction to form methane and hydrogen by a two-step proceduremechanism.

Research institute of innovative technology for earth proposed a global CO2

recycle system in which a solar power station installed in a desert to generate electricpower, and using this electric power, hydrogen gas was produced and used formethanol production [329]. The conversion of CO2 to methanol undergoes inpresence of Cu and Zn catalyst and further studies are underway to understand themechanism and to efficiently convert the mixtures to methanol [330–343].

Very few or comparatively less (Wrt oxidation) photo catalytic reduction studiesof CO2 by titania to hydrocarbon was experimented and was found to be effectivebased on the structures of the titania in presence and absence of moisture through theformation of carbonate/bicarbonates and formic acid [334]. The reduction processwas temperature dependent, where the reduction process was comparatively less at ahigher temperature and higher at lower temperatures. The reason for this might bedue to the collapse of the tubular nanostructures of TiNT under the coordinated Tisites [335]. Water is also found to influence the catalytic activity, as the waterprovides the protons needed for the conversion of CO2 to hydrocarbons. Further,the coordination of water molecule will potentially lower the energy barrier for thereaction to form the desired hydrocarbon product such as formic acid and methanol[336].

Sequestration using microalgae is one of the smartest ways to utilize the atmo-spheric gas for [337] improving the biomass of the microorganism at the same timereducing the CO2 level in the air. These microalgae in presence of water and sunlighttake CO2 to create biomass, which can be converted to value added products. Usingflue gas for growing microalgae for biofuel production was already reported, but itfaces some series technical challenges such as the cost involved in capturing theCO2, purifying it and then transportation. The CO2 required for the growth of thealgae was first converted to its respective bicarbonates, and these bicarbonates havebeen used as the culture medium and source of CO2 for the growth of algae.


Converting CO2 to bicarbonate increases the transport of CO2 much easier in thecells. Despite being the medium to transport CO2, these bicarbonates also increasesthe lipid accumulation in the cells of the algae which increases the biomass content,which is much useful for converting the biomass to value added products likebiofuels.

Albedo Modification

Albedo modification is the process of increasing the amount of scattered sunlight andreflecting it back to space thereby reducing the amount of sunlight absorbed by theearth, by injecting aerosols into the stratosphere, marine cloud brightening, andefforts to enhance surface reflectivity. Overview of difference between conventionalCO2 removal and albedo modification is given in Table 3.

Albedo modification has the potential to rapidly offset some of the globalwarming consequences at an affordable cost. If less energy is absorbed by theearth system, the earth’s surface is going to cool on an average, which is provenby the past volcanic eruptions which injected tons and tons of gases like sulfurdioxide into the stratosphere which acts as a blanket to reflect the sunlight causingthe reduction in the globally averaged surface air temperature to an estimate of 0.3Cfor a period of 3 years. Though the albedo process is rapid, it lasts only for theinterim time unto the ejected albedo is active.

Aerosols in the stratosphere can also bring in the reduction of incoming sunlight.The cost for this technology is much less than the technology for decarbonizing.

Table 3 Overview of difference between conventional CO2 removal and albedo modification

S.No. CO2 removal proposals Albedo modification proposals

1. Addresses the anthropogenic reasons for climaticchange which contribute to high atmosphericGHG concentration.

Do not consider the source of GHGand its impact on the climate

2. The proposals will not pose any risk factor Introduces global risk along with theproposal

3. Very expensive to be commissioned in industries Not expensive to implement

4. The effect of these proposals will take decades tosee a noticeable change

The effect will be seen within years ofimplementation

5. Raises fewer and less difficult issues with respectto global governance

Raise difficult issues with respect toglobal governance

6. The main factor will be the cost ofimplementation

The main factor will be the riskassociated with the proposal

7. Requires cooperation by major carbon emittersto have a significant effect

Could be done unilaterally

8. The proposal can be stopped after continuing forcertain years, but there won’t be any noticeableconsequence of dropping

If the project is abruptly terminated,there will be significant consequences


Some of the risks associated with albedo are ozone loss, changes in precipitation,and likely increased growth rates of forests caused by an increase in diffuse solarradiation; volcanic eruption may also lead to widespread crop failure and famine.There are many research opportunities in the field of albedo modification includingthe risk and benefits associated with implementing this process (see Fig. 10).

Future Perspectives and Conclusion

The progress till date was found to be slow but that is the first step in reducing thegreenhouse emission. The strange thing is all these slow processes are happeningonly in industrialized and developed countries and the other developing countriescontribution is very less, whose participation is more important to keep up the paceto fully eradicate the globally released CO2 in the atmosphere. Development of CCSprocess has to be done with the nonorganization for economic cooperation anddevelopment (non-OECD) countries, because these are the countries which willnot come into this OECD list, who will contribute to 70% of the emission by2050, led by China with a major share. The assessments and policies adopted bymultilateral development banks of OECD countries should work hand in hand withthe non-OECD countries to adopt the policies and establish the drive towardsdeployment of CCS globally. Cooperation among governments should be encour-aged widely which will ensure the global distribution of projects in order to cover the

Fig. 10 Albedo modification (Source: https://www.nasa.gov/images/content/574776main_StratoAerosolProcess-1600.jpg)


https://www.nasa.gov/images/content/574776main_StratoAerosolProcess-1600.jpg

https://www.nasa.gov/images/content/574776main_StratoAerosolProcess-1600.jpg

full spectrum of CCS application. Negative emission technologies have to beinformed to the society about the potential risk and opportunities afforded by allmitigation options in order to decide the desirable technology for the mitigation andtowards improvisation.

In this chapter, a brief description of the different processes commercialized andin the lab, the scale was discussed. The agreement and policies in order to reduce thealarming release of CO2 to the atmosphere were discussed along with the status ofthe developing and developed countries. Their mitigation process with the availabletechniques and raw materials ranging from Carbonaceous, Zeolite, Silica, CNT,MOF, Membranes, etc., were discussed. The problems revolving around sequestra-tion of the captured CO2 in bore wells and some of the value added products fromCO2 were also discussed. Albedo process towards reducing the global warming byscattering the incoming light was dealt in brief and the problem associated with it isinstalling. Overview of difference between conventional CO2 removal and albedomodification.

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https://doi.org/10.1073/pnas.1311316110

https://doi.org/10.1073/pnas.1311316110

https://www.chemistryworld.com/news/sun-shines-for-iron-catalyst-to-convert-carbon-dioxide-to-methane/3007722.article

https://www.chemistryworld.com/news/sun-shines-for-iron-catalyst-to-convert-carbon-dioxide-to-methane/3007722.article

https://doi.org/10.1016/0926-860X(95)00305-3

https://doi.org/10.1002/(SICI)1097-461X(2000)77:1<341::AID-QUA33>3.0.CO;2-T



https://doi.org/10.1016/0021-9517(87)90281-8

https://doi.org/10.1016/0021-9517(87)90281-8

https://doi.org/10.3390/molecules200915469

http://www.kscst.iisc.ernet.in/spp/38_series/spp38s/synopsis_biofuel/MSC/247_38S_B_MSc_015.pdf

http://www.kscst.iisc.ernet.in/spp/38_series/spp38s/synopsis_biofuel/MSC/247_38S_B_MSc_015.pdf

CO2 Sequestration: Processes and Methodologies...CCS Technologies ..... 15 Cryogenic Process ........

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