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  • P hD

    T he

    si s

    Tank designs for combined high-pressure gas and solid-state hydrogen storage

    Andrea Mazzucco DCAMM Special Report No. S197 January 2016

  • Tank designs for combined high pressure gas and solid state hydrogen storage

    PhD Thesis

    submitted the 31st January 2016

    and defended the 11th April 2016

    at the


    for the degree of Doctor of Philosophy


    Andrea Mazzucco

    under suggestion of:

    Associate Professor Masoud Rokni (DTU), main supervisor

    Associate Professor Brian Elmegaard (DTU), co-supervisor

    and under recommendation of:

    Professor Qingfeng Li (DTU), examiner

    Professor Volodymyr Yartys (NTNU), examiner

    Research scientist José M. Bellosta von Colbe (HZG), examiner

  • Tank designs for combined high pressure gas and solid state hydrogen storage

    Copyright ©2015 by Andrea Mazzucco. All rights reserved.

    PhD Thesis DCAMM Special Report no. S197

    Printed by Rosendahls – Schultz Grafisk A/S

    Font: Utopia typeset with LATEX 2ε

    DTU Mechanical Engineering Section of Thermal Energy Technical University of Denmark

    Nils Koppels Allé, Bld. 403

    DK-2800 Kongens Lyngby


    Phone: (+45) 45 25 41 31

    Fax: (+45) 45 25 43 25

    ISBN: 978-87-7475-443-5

  • to my family that has always been there for me

    and to my friends with whom I shared happiness and sorrow

  • Two roads diverged in a wood, and I – I took the one less traveled by,

    and that has made all the difference.

    — R. Frost, The road not taken

  • Preface

    The present thesis is submitted as a partial fulfillment of the requirements for the

    degree of Philosophiae Doctor (Ph.D.) at the Technical University of Denmark (DTU).

    The thesis was completed at the Section of Thermal Energy, Department of Mechani-

    cal Engineering. This work was carried out from the 1st of November 2012 to the 31st

    of January 2016 under the supervision of Associate Professor Masoud Rokni and the

    co-supervision of Associate Professor Brian Elmegaard.

    An external research stay was undertaken from April 2014 to September 2014 at the

    Hydrogen Systems Laboratory, an interdisciplinary facility of the Maurice J. Zucrow

    Laboratories at Purdue University in West Lafayette, Indiana, United States, under the

    supervision of Associate Professor Timothée L. Pourpoint.

    The Ph.D. study was funded by the Technical University of Denmark and the Danish

    Energy Agency through the Hyfill-Fast International Research Project in collaboration

    H2Logic as the inductrial partner. Financial support was also received from the Otto

    Mønsted A/S Fond in the frame of the WHEC 2014 and IGEC-X 2015 conferences and

    of the external research stay at Purdue University.

    The thesis is written in the form of a monograph and includes all the relevant publica-

    tions produced in the time frame of the present research study.

    Copenhagen, January 31st 2016

    Andrea Mazzucco


  • Acknowledgments

    It is hard to put into meaningful words my deep feeling of gratitude for all the people

    that have walked with me to the end of this journey.

    My attempt might result poor to most of the people that will read these pages, but at

    least, I will always have the profound awareness that these simple words are nothing

    but true.

    At first, I would like to thank the people at the university that have directly contributed

    to the work presented in this thesis. In particular, I would like to express my deepest

    gratitude to my supervisor, Professor Masoud Rokni, for his guidance and the numer-

    ous discussions we had in the past three years. I also thank him for giving me the

    opportunity to share a relationship of mutual confidence and respect. I am also very

    grateful to my co-supervisor Professor Brian Elmegaard for both the productive con-

    versations and the friendly working environment he managed to build at the section.

    It is hard not to thank all the members of the Hyfill-Fast International Research Project,

    including Michael Sloth from H2Logic for the many useful meetings and especially

    Jens-Erick Jørgensen and Torben Jensen at Aarhus University for their interesting

    inputs on novel research topics.

    My stay at Purdue University would not have been possible without Professor Timo-

    thée Pourpoint who accepted me in his laboratory and introduced me to his research

    team. I am also grateful to Tyler Voskuilen whose help was fundamental to the success

    of the work carried out during my external stay of research.

    A special thanks goes to all my friends in Denmark and abroad who supported me

    and with whom I shared moments of happiness and hard work. Lorenzo, for being the

    first who accepted me as a friend at the section and for cheering me up with jokes that

    will always leave a mark in my mind. Danilo, for his inspiring “joie de vivre” and his

    many attempts to teach me that being young is just a state of mind. Erasmus, for his

    warm friendship and for the help he was always ready to give me. Tuong-Van, whose

    name I will never be able to pronounce correctly, for proving himself a true friend over


  • Acknowledgments

    the years and for the many dinners shared at the office and downtown. Jorrit, for his

    cheerful spirit in the office and the nice moments spent together beyond the doors

    of the university. Torben, for the many beers and jokes. Leonardo for the convivial

    working environment.

    To Carlotta goes my profound gratitude for what is, without any doubt, the happiest

    time I had in Denmark. I wish you could have the same thorough confidence that I

    have on your success in any goals you will set for yourself and in any challenges you

    will brave in your future.

    At last, but not least I want to thank my family. My father Guido, my mother Cristina,

    my brother Luca and my beloved grandmother Pierina for being a reference point in

    my entire life and for all the support they gave me through these many years.


  • Abstract

    Many challenges have still to be overcome in order to establish a solid ground for

    significant market penetration of fuel cell hydrogen vehicles. The development of an

    effective solution for on-board hydrogen storage is one of the main technical tasks

    that need to be tackled.

    The present thesis deals with the development of a simulation tool to design and

    compare different vehicular storage options with respect to targets based upon stor-

    age and fueling efficiencies. The set targets represent performance improvements

    with regard to the state-of-the-art technology and are separately defined for each

    storage solution investigated in this work. Attention is given to solutions that involve

    high-pressure solid-state and gas hydrogen storage with an integrated passive cooling

    system. A set of libraries is implemented in the modeling platform to select among

    different material compositions, kinetic equations, heat exchanger configurations and

    to enable the tailoring of the analysis according to the user needs.

    Reliable computational models are developed to describe hydriding and dehydrid-

    ing reactions as well as melting and solidification processes that occur in the metal

    hydride tank and novel compressed-hydrogen vessel respectively. For the former,

    these models are used to quantify the main design parameter, being the critical metal

    hydride thickness, for the tank/heat-exchanger system.

    For the metal hydride tank, the tubular layout in a shell and tube configuration with 2

    mm inner diameter tubes is found to achieve the desired refueling time of 3 min and

    store a maximum of 3.1 kg of hydrogen in a 126 L tank. The dehydriding ability of this

    solution is proven to withstand intense discharging conditions.

    For the hydrogen gas tank, a novel design that includes a phase change material in

    its inner volume. Heat transfer augmentation techniques (e.g. encapsulation) are

    found to be the reward strategy to achieve the same stored mass and fueling time of

    the standard technology, while enabling ambient temperature fueling and save the

    energy cooling demand (4.2 MJ per fueling) at the refueling station.


  • Resumé

    For at skabe en solid base for et markedsgennembrud af brændselscellebiler er der sta-

    digvæk en del udfordringer der skal overkommes. Udviklingen af en tank der effektivt

    kan lagre brinten i køretøjet er en af de primære tekniske udfordringer som skal løses.

    Denne afhandling beskæftiger sig med udviklingen af et simuleringsværktøj der kan

    bruges til at sammenligne forskellige brintlagringsteknologier indenfor målene for

    lagring- og fyldningseffektivitet. De fastsatte mål repræsenterer forbedring i ydelse i

    forhold til den nyeste teknologi og de er forskelligt defineret for hver lagringstekno-

    logi. Fokus er lagt på løsninger der indebærer brint lagret som højtryksgas og brint

    bundet i fast stof, begge med et passivt kølesystem