Computationally Predicted High-Throughput Free-Energy Phase Diagrams for the Discovery of Solid-State Hydrogen Storage Reactions
Abstract
The design of multinary solid-state material systems that undergo reversible phase changes via changes in temperature and pressure provides a potential means of safely storing hydrogen. However, fully mapping the stabilities of known or newly targeted compounds relative to competing phases at reaction conditions has previously required many stringent experiments or computationally demanding calculations of each compound’s change in Gibbs energy with respect to temperature, G(T). Here, we have extended the approach of constructing chemical potential phase diagrams based on ΔGf(T) to enable the analysis of phase stability at non-zero temperatures. We first performed density functional theory calculations to compute the formation enthalpies of binary, ternary, and quaternary compounds within several compositional spaces of current interest for solid-state hydrogen storage. Temperature effects on solid compound stability were then accounted for using our recently introduced machine learned descriptor for the temperature-dependent contribution Gδ(T) to the Gibbs energy G(T). From these Gibbs energies, we evaluated each compound’s stability relative to competing compounds over a wide range of conditions and show using chemical potential and composition phase diagrams that the predicted stable phases and H2 release reactions are consistent with experimental observations. This demonstrates that our approach rapidly computes the thermochemistry of hydrogenmore »
- Authors:
-
- Univ. of Colorado, Boulder, CO (United States)
- Univ. of Colorado, Boulder, CO (United States); National Renewable Energy Lab. (NREL), Golden, CO (United States)
- Publication Date:
- Research Org.:
- National Renewable Energy Lab. (NREL), Golden, CO (United States); Energy Frontier Research Centers (EFRC) (United States). Center for Next Generation of Materials Design (CNGMD)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF); USDOE Office of Energy Efficiency and Renewable Energy (EERE), Transportation Office. Fuel Cell Technologies Office
- OSTI Identifier:
- 1710187
- Report Number(s):
- NREL/JA-5K00-78277
Journal ID: ISSN 1944-8244; MainId:32194;UUID:5504a162-b199-4185-a118-a63eeb63eb17;MainAdminID:18790
- Grant/Contract Number:
- AC36-08GO28308; CHEM 1800592; CBET 1806079; CBET 2016225; EE0008088
- Resource Type:
- Accepted Manuscript
- Journal Name:
- ACS Applied Materials and Interfaces
- Additional Journal Information:
- Journal Volume: 12; Journal Issue: 43; Journal ID: ISSN 1944-8244
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 08 HYDROGEN; free-energy phase diagrams; density functional theory; hydrogen storage; chemical potential; high-throughput; solid-state chemistry; thermodynamic stability
Citation Formats
Clary, Jacob M., Holder, Aaron M., and Musgrave, Charles B. Computationally Predicted High-Throughput Free-Energy Phase Diagrams for the Discovery of Solid-State Hydrogen Storage Reactions. United States: N. p., 2020.
Web. doi:10.1021/acsami.0c13298.
Clary, Jacob M., Holder, Aaron M., & Musgrave, Charles B. Computationally Predicted High-Throughput Free-Energy Phase Diagrams for the Discovery of Solid-State Hydrogen Storage Reactions. United States. https://doi.org/10.1021/acsami.0c13298
Clary, Jacob M., Holder, Aaron M., and Musgrave, Charles B. Mon .
"Computationally Predicted High-Throughput Free-Energy Phase Diagrams for the Discovery of Solid-State Hydrogen Storage Reactions". United States. https://doi.org/10.1021/acsami.0c13298. https://www.osti.gov/servlets/purl/1710187.
@article{osti_1710187,
title = {Computationally Predicted High-Throughput Free-Energy Phase Diagrams for the Discovery of Solid-State Hydrogen Storage Reactions},
author = {Clary, Jacob M. and Holder, Aaron M. and Musgrave, Charles B.},
abstractNote = {The design of multinary solid-state material systems that undergo reversible phase changes via changes in temperature and pressure provides a potential means of safely storing hydrogen. However, fully mapping the stabilities of known or newly targeted compounds relative to competing phases at reaction conditions has previously required many stringent experiments or computationally demanding calculations of each compound’s change in Gibbs energy with respect to temperature, G(T). Here, we have extended the approach of constructing chemical potential phase diagrams based on ΔGf(T) to enable the analysis of phase stability at non-zero temperatures. We first performed density functional theory calculations to compute the formation enthalpies of binary, ternary, and quaternary compounds within several compositional spaces of current interest for solid-state hydrogen storage. Temperature effects on solid compound stability were then accounted for using our recently introduced machine learned descriptor for the temperature-dependent contribution Gδ(T) to the Gibbs energy G(T). From these Gibbs energies, we evaluated each compound’s stability relative to competing compounds over a wide range of conditions and show using chemical potential and composition phase diagrams that the predicted stable phases and H2 release reactions are consistent with experimental observations. This demonstrates that our approach rapidly computes the thermochemistry of hydrogen release reactions for compounds at sufficiently high accuracy relative to experiment to provide a powerful framework for analyzing hydrogen storage materials. This framework based on G(T) enables the accelerated discovery of active materials for a variety of technologies that rely on solid-state reactions involving these materials.},
doi = {10.1021/acsami.0c13298},
journal = {ACS Applied Materials and Interfaces},
number = 43,
volume = 12,
place = {United States},
year = {Mon Oct 19 00:00:00 EDT 2020},
month = {Mon Oct 19 00:00:00 EDT 2020}
}
Works referenced in this record:
Synthesis and hydriding properties of Li2Mg(NH)2
journal, April 2010
- Markmaitree, Tippawan; Shaw, Leon L.
- Journal of Power Sources, Vol. 195, Issue 7
Analysis of the Electronic Structure of Modified CuGaS 2 with Selected Substitutional Impurities: Prospects for Intermediate-Band Thin-Film Solar Cells Based on Cu-Containing Chalcopyrites
journal, January 2010
- Tablero, C.; Fuertes Marrón, D.
- The Journal of Physical Chemistry C, Vol. 114, Issue 6
Hydrogen storage properties in Ti catalyzed Li–N–H system
journal, December 2005
- Ichikawa, T.; Hanada, N.; Isobe, S.
- Journal of Alloys and Compounds, Vol. 404-406
First-Principles Determination of Multicomponent Hydride Phase Diagrams: Application to the Li-Mg-N-H System
journal, September 2007
- R. Akbarzadeh, A.; Ozoliņš, V.; Wolverton, C.
- Advanced Materials, Vol. 19, Issue 20
Desorption characteristics of mechanically and chemically modified LiNH2 and (LiNH2+LiH)
journal, April 2007
- Yao, J. H.; Shang, C.; Aguey-Zinsou, K. F.
- Journal of Alloys and Compounds, Vol. 432, Issue 1-2
Potential of Binary Lithium Magnesium Nitride for Hydrogen Storage Applications
journal, July 2007
- Lu, Jun; Fang, Zhigang Zak; Choi, Young Joon
- The Journal of Physical Chemistry C, Vol. 111, Issue 32
Theoretical Prediction of Metastable Intermediates in the Decomposition of Mg(BH 4 ) 2
journal, May 2012
- Zhang, Yongsheng; Majzoub, Eric; Ozoliņš, Vidvuds
- The Journal of Physical Chemistry C, Vol. 116, Issue 19
Mg–Ti nanoparticles with superior kinetics for hydrogen storage
journal, August 2016
- Calizzi, Marco; Chericoni, Domizia; Jepsen, Lars H.
- International Journal of Hydrogen Energy, Vol. 41, Issue 32
Interaction of hydrogen with metal nitrides and imides
journal, November 2002
- Chen, Ping; Xiong, Zhitao; Luo, Jizhong
- Nature, Vol. 420, Issue 6913, p. 302-304
A review on the current progress of metal hydrides material for solid-state hydrogen storage applications
journal, July 2016
- Rusman, N. A. A.; Dahari, M.
- International Journal of Hydrogen Energy, Vol. 41, Issue 28
Ammonia synthesis at low temperatures
journal, March 2000
- Rod, T. H.; Logadottir, A.; Nørskov, J. K.
- The Journal of Chemical Physics, Vol. 112, Issue 12
The reaction pathway and rate-limiting step of dehydrogenation of the LiHN2+LiH mixture
journal, March 2008
- Shaw, Leon L.; Osborn, William; Markmaitree, Tippawan
- Journal of Power Sources, Vol. 177, Issue 2
The kinetics of lightweight solid-state hydrogen storage materials: A review
journal, August 2016
- Abd. Khalim Khafidz, Nurul Zafirah; Yaakob, Zahira; Lim, Kean Long
- International Journal of Hydrogen Energy, Vol. 41, Issue 30
Enhanced Hydrogen Storage Properties of Li−Mg−N−H System Prepared by Reacting Mg(NH 2 ) 2 with Li 3 N
journal, May 2009
- Ma, Lai-Peng; Dai, Hong-Bin; Fang, Zhan-Zhao
- The Journal of Physical Chemistry C, Vol. 113, Issue 22
Physiochemical Pathway for Cyclic Dehydrogenation and Rehydrogenation of LiAlH 4
journal, May 2006
- Wang, Jun; Ebner, Armin D.; Ritter, James A.
- Journal of the American Chemical Society, Vol. 128, Issue 17
GW self-energy calculations for surfaces and interfaces
journal, June 2001
- Garcı́a-González, P.; Godby, R. W.
- Computer Physics Communications, Vol. 137, Issue 1
Recent advances in improving performances of the lightweight complex hydrides Li-Mg-N-H system
journal, February 2017
- Zhang, Bao; Wu, Ying
- Progress in Natural Science: Materials International, Vol. 27, Issue 1
Destabilization and enhanced dehydriding reaction of LiNH2: an electronic structure viewpoint
journal, November 2004
- Orimo, S.; Nakamori, Y.; Kitahara, G.
- Applied Physics A, Vol. 79, Issue 7
Li–Mg–N–H-based combination systems for hydrogen storage
journal, July 2011
- Liang, Chu; Liu, Yongfeng; Fu, Hongliang
- Journal of Alloys and Compounds, Vol. 509, Issue 30
Interaction between Lithium Amide and Lithium Hydride
journal, October 2003
- Chen, Ping; Xiong, Zhitao; Luo, Jizhong
- The Journal of Physical Chemistry B, Vol. 107, Issue 39, p. 10967-10970
Correcting density functional theory for accurate predictions of compound enthalpies of formation: Fitted elemental-phase reference energies
journal, March 2012
- Stevanović, Vladan; Lany, Stephan; Zhang, Xiuwen
- Physical Review B, Vol. 85, Issue 11
USPEX—Evolutionary crystal structure prediction
journal, December 2006
- Glass, Colin W.; Oganov, Artem R.; Hansen, Nikolaus
- Computer Physics Communications, Vol. 175, Issue 11-12
Ternary Imides for Hydrogen Storage
journal, September 2004
- Xiong, Z.; Wu, G.; Hu, J.
- Advanced Materials, Vol. 16, Issue 17
Complex hydrides for hydrogen storage – new perspectives
journal, April 2014
- Ley, Morten B.; Jepsen, Lars H.; Lee, Young-Su
- Materials Today, Vol. 17, Issue 3
Ab Initio Thermochemistry of Solid-State Materials
journal, June 2010
- Stoffel, Ralf Peter; Wessel, Claudia; Lumey, Marck-Willem
- Angewandte Chemie International Edition, Vol. 49, Issue 31
A Mechanism for Non-stoichiometry in the Lithium Amide/Lithium Imide Hydrogen Storage Reaction
journal, February 2007
- David, William I. F.; Jones, Martin O.; Gregory, Duncan H.
- Journal of the American Chemical Society, Vol. 129, Issue 6
Understanding the Decomposition Mechanisms of LiNH 2 , Mg(NH 2 ) 2 , and NaNH 2 : A Joint Experimental and Theoretical Study
journal, July 2019
- Lin, Huai-Jun; Zhang, Peng; Fang, Yan-Xiong
- The Journal of Physical Chemistry C, Vol. 123, Issue 30
Dehydrogenation reaction of Li–Mg–N–H systems studied by in situ synchrotron powder X-ray diffraction and powder neutron diffraction
journal, June 2008
- Nakamura, Y.; Hino, S.; Ichikawa, T.
- Journal of Alloys and Compounds, Vol. 457, Issue 1-2
The Open Quantum Materials Database (OQMD): assessing the accuracy of DFT formation energies
journal, December 2015
- Kirklin, Scott; Saal, James E.; Meredig, Bryce
- npj Computational Materials, Vol. 1, Issue 1
The Role of Free N-Heterocyclic Carbene (NHC) in the Catalytic Dehydrogenation of Ammonia-Borane in the Nickel NHC System
journal, March 2009
- Zimmerman, Paul M.; Paul, Ankan; Zhang, Zhiyong
- Angewandte Chemie International Edition, Vol. 48, Issue 12
Efficiency of ab-initio total energy calculations for metals and semiconductors using a plane-wave basis set
journal, July 1996
- Kresse, G.; Furthmüller, J.
- Computational Materials Science, Vol. 6, Issue 1, p. 15-50
Studies on dehydrogenation characteristic of Mg(NH2)2/LiH mixture admixed with vanadium and vanadium based catalysts (V, V2O5 and VCl3)
journal, January 2010
- Shahi, Rohit R.; Yadav, T. P.; Shaz, M. A.
- International Journal of Hydrogen Energy, Vol. 35, Issue 1
Ultrafast Reaction between LiH and NH 3 during H 2 Storage in Li 3 N
journal, November 2003
- Hu, Yun Hang; Ruckenstein, Eli
- The Journal of Physical Chemistry A, Vol. 107, Issue 46
Physical descriptor for the Gibbs energy of inorganic crystalline solids and temperature-dependent materials chemistry
journal, October 2018
- Bartel, Christopher J.; Millican, Samantha L.; Deml, Ann M.
- Nature Communications, Vol. 9, Issue 1
Structural and Compositional Changes during Hydrogenation/Dehydrogenation of the Li−Mg−N−H System
journal, December 2007
- Hu, Jianjiang; Liu, Yongfeng; Wu, Guotao
- The Journal of Physical Chemistry C, Vol. 111, Issue 49
High H 2 Uptake in Li-, Na-, K-Metalated Covalent Organic Frameworks and Metal Organic Frameworks at 298 K
journal, February 2012
- Mendoza-Cortés, José L.; Han, Sang Soo; Goddard, William A.
- The Journal of Physical Chemistry A, Vol. 116, Issue 6
Catalyzed Dehydrogenation of Ammonia–Borane by Iridium Dihydrogen Pincer Complex Differs from Ethane Dehydrogenation
journal, November 2007
- Paul, Ankan; Musgrave, Charles B.
- Angewandte Chemie International Edition, Vol. 46, Issue 43
Commentary: The Materials Project: A materials genome approach to accelerating materials innovation
journal, July 2013
- Jain, Anubhav; Ong, Shyue Ping; Hautier, Geoffroy
- APL Materials, Vol. 1, Issue 1
Ti-doped alkali metal aluminium hydrides as potential novel reversible hydrogen storage materials
journal, May 1997
- Bogdanović, Borislav; Schwickardi, Manfred
- Journal of Alloys and Compounds, Vol. 253-254, p. 1-9
Thermogravimetric Measurement of Hydrogen Absorption in Alkali-Modified Carbon Materials
journal, October 2000
- Pinkerton, F. E.; Wicke, B. G.; Olk, C. H.
- The Journal of Physical Chemistry B, Vol. 104, Issue 40
Li–N based hydrogen storage materials
journal, April 2004
- Nakamori, Y.; Orimo, S.
- Materials Science and Engineering: B, Vol. 108, Issue 1-2
Improving Hydrogen Storage Capacity of MOF by Functionalization of the Organic Linker with Lithium Atoms
journal, June 2008
- Klontzas, Emmanouel; Mavrandonakis, Andreas; Tylianakis, Emmanuel
- Nano Letters, Vol. 8, Issue 6
First-Principles Screening of Complex Transition Metal Hydrides for High Temperature Applications
journal, October 2014
- Nicholson, Kelly M.; Sholl, David S.
- Inorganic Chemistry, Vol. 53, Issue 22
Hydrogen storage behaviour of Li3N doped with Li2O and Na2O
journal, April 2010
- Langmi, Henrietta W.; Culligan, Scott D.; McGrady, G. Sean
- Journal of Power Sources, Vol. 195, Issue 7
The role of decomposition reactions in assessing first-principles predictions of solid stability
journal, January 2019
- Bartel, Christopher J.; Weimer, Alan W.; Lany, Stephan
- npj Computational Materials, Vol. 5, Issue 1
(LiNH2–MgH2): a viable hydrogen storage system
journal, November 2004
- Luo, Weifang
- Journal of Alloys and Compounds, Vol. 381, Issue 1-2
Dehydrogenation kinetics of magnesium hydride investigated by DFT and experiment
journal, July 2010
- Wu, Guangxin; Zhang, Jieyu; Li, Qian
- Computational Materials Science, Vol. 49, Issue 1
Catalytic effect of halide additives ball milled with magnesium hydride
journal, February 2010
- Malka, I. E.; Czujko, T.; Bystrzycki, J.
- International Journal of Hydrogen Energy, Vol. 35, Issue 4
Magnetism without Magnetic Ions: Percolation, Exchange, and Formation Energies of Magnetism-Promoting Intrinsic Defects in CaO
journal, March 2006
- Osorio-Guillén, J.; Lany, S.; Barabash, S. V.
- Physical Review Letters, Vol. 96, Issue 10
Crystal structure prediction using ab initio evolutionary techniques: Principles and applications
journal, June 2006
- Oganov, Artem R.; Glass, Colin W.
- The Journal of Chemical Physics, Vol. 124, Issue 24
Reversible hydrogen-storage functions for mixtures of Li3N and Mg3N2
journal, January 2005
- Nakamori, Y.; Kitahara, G.; Miwa, K.
- Applied Physics A, Vol. 80, Issue 1
Improved kinetics of the Mg(NH 2 ) 2 –2LiH system by addition of lithium halides
journal, January 2014
- Cao, Hujun; Wang, Han; He, Teng
- RSC Advances, Vol. 4, Issue 61
Catalytic Dehydrogenation of Ammonia Borane at Ni Monocarbene and Dicarbene Catalysts
journal, June 2009
- Zimmerman, Paul M.; Paul, Ankan; Musgrave, Charles B.
- Inorganic Chemistry, Vol. 48, Issue 12