A Computational Framework to Accelerate the Discovery of Perovskites for Solar Thermochemical Hydrogen Production: Identification of Gd Perovskite Oxide Redox Mediators

Bare, Zachary L.; Morelock, Ryan J.; Musgrave, Charles B.

doi:10.1002/adfm.202200201

A Computational Framework to Accelerate the Discovery of Perovskites for Solar Thermochemical Hydrogen Production: Identification of Gd Perovskite Oxide Redox Mediators

Journal Article · Sun Mar 20 00:00:00 EDT 2022 · Advanced Functional Materials

DOI:https://doi.org/10.1002/adfm.202200201· OSTI ID:1976187

Bare, Zachary L. ^[1]; Morelock, Ryan J. ^[2]; ^[2]

University of Colorado, Boulder, CO (United States); OSTI
University of Colorado, Boulder, CO (United States)

A high-throughput computational framework to identify novel multinary perovskite redox mediators is presented, and this framework is applied to discover the Gd-containing perovskite oxide compositions Gd₂BB'O₆, GdA'B₂O₆, and GdA'BB'O₆ that split water. The computational scheme uses a sequence of empirical approaches to evaluate the stabilities, electronic properties, and oxygen vacancy thermodynamics of these materials, including contributions to the enthalpies and entropies of reduction, ΔH_TR and ΔS_TR. This scheme uses the machine-learned descriptor τ to identify compositions that are likely stable as perovskites, the bond valence method to estimate the magnitude and phase of BO₆ octahedral tilting and provide accurate initial estimates of perovskite geometries, and density functional theory including magnetic- and defect-sampling to predict STCH-relevant properties. Eighty-three promising STCH candidate perovskite oxides down-selected from 4392 Gd-containing compositions are reported, three of which are referred to experimental collaborators for characterization and exhibit STCH activity. Our results demonstrate that the high-throughput computational scheme described herein—which is used to evaluate Gd-containing compositions but can be applied to any multinary perovskite oxide compositional space(s) of interest—accelerates the discovery of novel STCH active redox mediators with reasonable computational expense.

View Accepted Manuscript (DOE)

Research Organization:: University of Colorado, Boulder, CO (United States)

Sponsoring Organization:: National Science Foundation (NSF); USDOE; USDOE Office of Energy Efficiency and Renewable Energy (EERE), Office of Sustainable Transportation. Hydrogen Fuel Cell Technologies Office (HFTO); University of Colorado

Grant/Contract Number:: EE0008088

OSTI ID:: 1976187

Alternate ID(s):: OSTI ID: 1856536

Journal Information:: Advanced Functional Materials, Journal Name: Advanced Functional Materials Journal Issue: 25 Vol. 32; ISSN 1616-301X

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

References (61)

The Hiphive Package for the Extraction of High‐Order Force Constants by Machine Learning Eriksson, Fredrik; Fransson, Erik; Erhart, Paul Advanced Theory and Simulations, Vol. 2, Issue 5 https://doi.org/10.1002/adts.201800184	journal	February 2019
Considerations in the Design of Materials for Solar-Driven Fuel Production Using Metal-Oxide Thermochemical Cycles Miller, James E.; McDaniel, Anthony H.; Allendorf, Mark D. Advanced Energy Materials, Vol. 4, Issue 2, Article No. 1300469 https://doi.org/10.1002/aenm.201300469	journal	October 2013
Ln _0.5 A _0.5 MnO ₃ (Ln=Lanthanide, A= Ca, Sr) Perovskites Exhibiting Remarkable Performance in the Thermochemical Generation of CO and H ₂ from CO ₂ and H ₂ O Dey, Sunita; Naidu, B. S.; Rao, C. N. R. Chemistry - A European Journal, Vol. 21, Issue 19 https://doi.org/10.1002/chem.201500442	journal	March 2015
Towards Solar Fuels from Water and CO ₂ Centi, Gabriele; Perathoner, Siglinda ChemSusChem, Vol. 3, Issue 2 https://doi.org/10.1002/cssc.200900289	journal	February 2010
A review and perspective of efficient hydrogen generation via solar thermal water splitting: A review and perspective of efficient hydrogen generation Muhich, Christopher L.; Ehrhart, Brian D.; Al-Shankiti, Ibraheam Wiley Interdisciplinary Reviews: Energy and Environment, Vol. 5, Issue 3 https://doi.org/10.1002/wene.174	journal	May 2015
Cerium ion redox system in CeO2–xFe2O3 solid solution at high temperatures (1,273–1,673 K) in the two-step water-splitting reaction for solar H2 generation Kaneko, H.; Ishihara, H.; Taku, S. Journal of Materials Science, Vol. 43, Issue 9 https://doi.org/10.1007/s10853-008-2499-z	journal	May 2008
Hydrogen production from water utilizing solar heat at high temperatures Nakamura, T. Solar Energy, Vol. 19, Issue 5 https://doi.org/10.1016/0038-092X(77)90102-5	journal	January 1977
Efficiency of ab-initio total energy calculations for metals and semiconductors using a plane-wave basis set Kresse, G.; Furthmüller, J. Computational Materials Science, Vol. 6, Issue 1, p. 15-50 https://doi.org/10.1016/0927-0256(96)00008-0	journal	July 1996
Solar hydrogen production via a two-step water-splitting thermochemical cycle based on Zn/ZnO redox reactions Steinfeld, A. International Journal of Hydrogen Energy, Vol. 27, Issue 6, p. 611-619 https://doi.org/10.1016/S0360-3199(01)00177-X	journal	June 2002
Python Materials Genomics (pymatgen): A robust, open-source python library for materials analysis Ong, Shyue Ping; Richards, William Davidson; Jain, Anubhav Computational Materials Science, Vol. 68 https://doi.org/10.1016/j.commatsci.2012.10.028	journal	February 2013
Nonstoichiometric Perovskite Oxides for Solar Thermochemical H2 and CO Production McDaniel, A. H.; Ambrosini, A.; Coker, E. N. Energy Procedia, Vol. 49 https://doi.org/10.1016/j.egypro.2014.03.213	journal	January 2014
Comparing the solar-to-fuel energy conversion efficiency of ceria and perovskite based thermochemical redox cycles for splitting H2O and CO2 Muhich, Christopher L.; Blaser, Samuel; Hoes, Marie C. International Journal of Hydrogen Energy, Vol. 43, Issue 41 https://doi.org/10.1016/j.ijhydene.2018.08.137	journal	October 2018
Double perovskite anti-supported rare earth oxide catalyst CeO2/La2CoFeO6 for efficient ventilation air methane combustion Gao, Xiaojiao; Jin, Zehua; Hu, Ruisheng Journal of Rare Earths, Vol. 39, Issue 4 https://doi.org/10.1016/j.jre.2020.07.022	journal	April 2021
Outstanding Properties and Performance of CaTi0.5Mn0.5O3–δ for Solar-Driven Thermochemical Hydrogen Production Qian, Xin; He, Jiangang; Mastronardo, Emanuela Matter, Vol. 4, Issue 2 https://doi.org/10.1016/j.matt.2020.11.016	journal	February 2021
Solar thermochemical production of hydrogen––a review Steinfeld, Aldo Solar Energy, Vol. 78, Issue 5, p. 603-615 https://doi.org/10.1016/j.solener.2003.12.012	journal	May 2005
Thermochemical hydrogen production from a two-step solar-driven water-splitting cycle based on cerium oxides Abanades, Stéphane; Flamant, Gilles Solar Energy, Vol. 80, Issue 12 https://doi.org/10.1016/j.solener.2005.12.005	journal	December 2006
Exploring Ca–Ce–M–O (M = 3d Transition Metal) Oxide Perovskites for Solar Thermochemical Applications Sai Gautam, Gopalakrishnan; Stechel, Ellen B.; Carter, Emily A. Chemistry of Materials, Vol. 32, Issue 23 https://doi.org/10.1021/acs.chemmater.0c02912	journal	November 2020
Favorable Redox Thermodynamics of SrTi _0.5 Mn _0.5 O _3−δ in Solar Thermochemical Water Splitting Qian, Xin; He, Jiangang; Mastronardo, Emanuela Chemistry of Materials, Vol. 32, Issue 21 https://doi.org/10.1021/acs.chemmater.0c03278	journal	October 2020
Phase Identification of the Layered Perovskite Ce _x Sr _{2– x} MnO ₄ and Application for Solar Thermochemical Water Splitting Barcellos, Debora R.; Coury, Francisco G.; Emery, Antoine Inorganic Chemistry, Vol. 58, Issue 12 https://doi.org/10.1021/acs.inorgchem.8b03487	journal	May 2019
Intrinsic Material Properties Dictating Oxygen Vacancy Formation Energetics in Metal Oxides Deml, Ann M.; Holder, Aaron M.; O’Hayre, Ryan P. The Journal of Physical Chemistry Letters, Vol. 6, Issue 10 https://doi.org/10.1021/acs.jpclett.5b00710	journal	May 2015
CeTi ₂ O ₆ —A Promising Oxide for Solar Thermochemical Hydrogen Production Naghavi, S. Shahab; He, Jiangang; Wolverton, C. ACS Applied Materials & Interfaces, Vol. 12, Issue 19 https://doi.org/10.1021/acsami.0c01083	journal	April 2020
Tunable Oxygen Vacancy Formation Energetics in the Complex Perovskite Oxide Sr _x La _{1– x} Mn _y Al _{1– y} O ₃ Deml, Ann M.; Stevanović, Vladan; Holder, Aaron M. Chemistry of Materials, Vol. 26, Issue 22 https://doi.org/10.1021/cm5033755	journal	November 2014
Lanthanum–Strontium–Manganese Perovskites as Redox Materials for Solar Thermochemical Splitting of H ₂ O and CO ₂ Scheffe, Jonathan R.; Weibel, David; Steinfeld, Aldo Energy & Fuels, Vol. 27, Issue 8 https://doi.org/10.1021/ef301923h	journal	March 2013
Factors Affecting the Efficiency of Solar Driven Metal Oxide Thermochemical Cycles Siegel, Nathan P.; Miller, James E.; Ermanoski, Ivan Industrial & Engineering Chemistry Research, Vol. 52, Issue 9, p. 3276-3286 https://doi.org/10.1021/ie400193q	journal	February 2013
FeO ₆ Octahedral Distortion Activates Lattice Oxygen in Perovskite Ferrite for Methane Partial Oxidation Coupled with CO ₂ Splitting Zhang, Xianhua; Pei, Chunlei; Chang, Xin Journal of the American Chemical Society, Vol. 142, Issue 26 https://doi.org/10.1021/jacs.0c04643	journal	June 2020
Inorganic Halide Double Perovskites with Optoelectronic Properties Modulated by Sublattice Mixing Bartel, Christopher J.; Clary, Jacob M.; Sutton, Christopher Journal of the American Chemical Society, Vol. 142, Issue 11 https://doi.org/10.1021/jacs.9b12440	journal	February 2020
Origin of ferroelectricity in perovskite oxides Cohen, Ronald E. Nature, Vol. 358, Issue 6382 https://doi.org/10.1038/358136a0	journal	July 1992
Giant onsite electronic entropy enhances the performance of ceria for water splitting Naghavi, S. Shahab; Emery, Antoine A.; Hansen, Heine A. Nature Communications, Vol. 8, Issue 1 https://doi.org/10.1038/s41467-017-00381-2	journal	August 2017
High-throughput DFT calculations of formation energy, stability and oxygen vacancy formation energy of ABO3 perovskites Emery, Antoine A.; Wolverton, Chris Scientific Data, Vol. 4, Issue 1 https://doi.org/10.1038/sdata.2017.153	journal	October 2017
Thermodynamic and kinetic assessments of strontium-doped lanthanum manganite perovskites for two-step thermochemical water splitting Yang, Chih-Kai; Yamazaki, Yoshihiro; Aydin, Aykut J. Mater. Chem. A, Vol. 2, Issue 33 https://doi.org/10.1039/C4TA02694B	journal	January 2014
Tunable thermodynamic activity of La _x Sr _1−x Mn _y Al _1−y O _3−δ (0 ≤ x ≤ 1, 0 ≤ y ≤ 1) perovskites for solar thermochemical fuel synthesis Ezbiri, M.; Takacs, M.; Theiler, D. Journal of Materials Chemistry A, Vol. 5, Issue 8 https://doi.org/10.1039/C6TA06644E	journal	January 2017
Perovskite oxides – a review on a versatile material class for solar-to-fuel conversion processes Kubicek, Markus; Bork, Alexander H.; Rupp, Jennifer L. M. Journal of Materials Chemistry A, Vol. 5, Issue 24 https://doi.org/10.1039/C7TA00987A	journal	January 2017
Applications and limitations of two step metal oxide thermochemical redox cycles; a review Bulfin, B.; Vieten, J.; Agrafiotis, C. Journal of Materials Chemistry A, Vol. 5, Issue 36 https://doi.org/10.1039/C7TA05025A	journal	January 2017
BaCe 0.25 Mn 0.75 O 3−δ —a promising perovskite-type oxide for solar thermochemical hydrogen production R. Barcellos, Debora; Sanders, Michael D.; Tong, Jianhua Energy & Environmental Science, Vol. 11, Issue 11 https://doi.org/10.1039/C8EE01989D	journal	January 2018
Materials design of perovskite solid solutions for thermochemical applications Vieten, Josua; Bulfin, Brendan; Huck, Patrick Energy & Environmental Science, Vol. 12, Issue 4 https://doi.org/10.1039/C9EE00085B	journal	January 2019
Commentary: The Materials Project: A materials genome approach to accelerating materials innovation Jain, Anubhav; Ong, Shyue Ping; Hautier, Geoffroy APL Materials, Vol. 1, Issue 1 https://doi.org/10.1063/1.4812323	journal	July 2013
Communication: The electronic entropy of charged defect formation and its impact on thermochemical redox cycles Lany, Stephan The Journal of Chemical Physics, Vol. 148, Issue 7 https://doi.org/10.1063/1.5022176	journal	February 2018
Low-temperature, manganese oxide-based, thermochemical water splitting cycle Xu, B.; Bhawe, Y.; Davis, M. E. Proceedings of the National Academy of Sciences, Vol. 109, Issue 24 https://doi.org/10.1073/pnas.1206407109	journal	May 2012
Solar thermochemical splitting of water to generate hydrogen Rao, C. N. R.; Dey, Sunita Proceedings of the National Academy of Sciences, Vol. 114, Issue 51 https://doi.org/10.1073/pnas.1700104114	journal	May 2017
Complementary evaluation of structure stability of perovskite oxides using bond-valence and density-functional-theory calculations Yamada, Ikuya; Takamatsu, Akihiko; Ikeno, Hidekazu Science and Technology of Advanced Materials, Vol. 19, Issue 1 https://doi.org/10.1080/14686996.2018.1430449	journal	February 2018
Determination of B-site ordering and structural transformations in the mixed transition metal perovskites La ₂ CoMnO ₆ and La ₂ NiMnO ₆ Bull, C. L.; Gleeson, D.; Knight, K. S. Journal of Physics: Condensed Matter, Vol. 15, Issue 29 https://doi.org/10.1088/0953-8984/15/29/304	journal	July 2003
Crystal structure and magnetic ordering of the LaCo _{1− x} Fe _x O ₃ system Karpinsky, D. V.; Troyanchuk, I. O.; Bärner, K. Journal of Physics: Condensed Matter, Vol. 17, Issue 46 https://doi.org/10.1088/0953-8984/17/46/006	journal	November 2005
Norm-conserving and ultrasoft pseudopotentials for first-row and transition elements Kresse, G.; Hafner, J. Journal of Physics: Condensed Matter, Vol. 6, Issue 40 https://doi.org/10.1088/0953-8984/6/40/015	journal	October 1994
Generation of low-symmetry perovskite structures for ab initio computation Xie, N.; Zhang, J.; Raza, S. Journal of Physics: Condensed Matter, Vol. 32, Issue 31 https://doi.org/10.1088/1361-648X/ab7f6a	journal	May 2020
Polymorphous nature of cubic halide perovskites Zhao, Xin-Gang; Dalpian, Gustavo M.; Wang, Zhi Physical Review B, Vol. 101, Issue 15 https://doi.org/10.1103/PhysRevB.101.155137	journal	April 2020
Ab initiomolecular dynamics for liquid metals Kresse, G.; Hafner, J. Physical Review B, Vol. 47, Issue 1, p. 558-561 https://doi.org/10.1103/PhysRevB.47.558	journal	January 1993
Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set Kresse, G.; Furthmüller, J. Physical Review B, Vol. 54, Issue 16, p. 11169-11186 https://doi.org/10.1103/PhysRevB.54.11169	journal	October 1996
From ultrasoft pseudopotentials to the projector augmented-wave method Kresse, G.; Joubert, D. Physical Review B, Vol. 59, Issue 3, p. 1758-1775 https://doi.org/10.1103/PhysRevB.59.1758	journal	January 1999
Oxidation energies of transition metal oxides within the GGA + U framework Wang, Lei; Maxisch, Thomas; Ceder, Gerbrand Physical Review B, Vol. 73, Issue 19 https://doi.org/10.1103/PhysRevB.73.195107	journal	May 2006
First-principles thermodynamic framework for the evaluation of thermochemical H 2 O - or CO 2 -splitting materials Meredig, B.; Wolverton, C. Physical Review B, Vol. 80, Issue 24 https://doi.org/10.1103/PhysRevB.80.245119	journal	December 2009
Correcting density functional theory for accurate predictions of compound enthalpies of formation: Fitted elemental-phase reference energies Stevanović, Vladan; Lany, Stephan; Zhang, Xiuwen Physical Review B, Vol. 85, Issue 11 https://doi.org/10.1103/PhysRevB.85.115104	journal	March 2012
Accuracy of density functional theory in predicting formation energies of ternary oxides from binary oxides and its implication on phase stability Hautier, Geoffroy; Ong, Shyue Ping; Jain, Anubhav Physical Review B, Vol. 85, Issue 15 https://doi.org/10.1103/PhysRevB.85.155208	journal	April 2012
Ab initio thermodynamics of intrinsic oxygen vacancies in ceria Gopal, Chirranjeevi Balaji; van de Walle, Axel Physical Review B, Vol. 86, Issue 13 https://doi.org/10.1103/PhysRevB.86.134117	journal	October 2012
Generalized Gradient Approximation Made Simple Perdew, John P.; Burke, Kieron; Ernzerhof, Matthias Physical Review Letters, Vol. 77, Issue 18, p. 3865-3868 https://doi.org/10.1103/PhysRevLett.77.3865	journal	October 1996
Prediction of the crystal structures of perovskites using the software program SPuDS Lufaso, Michael W.; Woodward, Patrick M. Acta Crystallographica Section B Structural Science, Vol. 57, Issue 6 https://doi.org/10.1107/S0108768101015282	journal	November 2001
Structural stability and formability of AB O ₃ -type perovskite compounds Zhang, Huan; Li, Na; Li, Keyan Acta Crystallographica Section B Structural Science, Vol. 63, Issue 6 https://doi.org/10.1107/S0108768107046174	journal	November 2007
Revised effective ionic radii and systematic studies of interatomic distances in halides and chalcogenides Shannon, R. D. Acta Crystallographica Section A, Vol. 32, Issue 5, p. 751-767 https://doi.org/10.1107/S0567739476001551	journal	September 1976
The classification of tilted octahedra in perovskites Glazer, A. M. Acta Crystallographica Section B Structural Crystallography and Crystal Chemistry, Vol. 28, Issue 11 https://doi.org/10.1107/S0567740872007976	journal	November 1972
New tolerance factor to predict the stability of perovskite oxides and halides Bartel, Christopher J.; Sutton, Christopher; Goldsmith, Bryan R. Science Advances, Vol. 5, Issue 2 https://doi.org/10.1126/sciadv.aav0693	journal	February 2019
Efficient Generation of H2 by Splitting Water with an Isothermal Redox Cycle Muhich, C. L.; Evanko, B. W.; Weston, K. C. Science, Vol. 341, Issue 6145 https://doi.org/10.1126/science.1239454	journal	August 2013
Computationally Accelerated Discovery and Experimental Demonstration of Gd0.5La0.5Co0.5Fe0.5O3 for Solar Thermochemical Hydrogen Production Park, James Eujin; Bare, Zachary J. L.; Morelock, Ryan J. Frontiers in Energy Research, Vol. 9 https://doi.org/10.3389/fenrg.2021.750600	journal	October 2021

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A Computational Framework to Accelerate the Discovery of Perovskites for Solar Thermochemical Hydrogen Production: Identification of Gd Perovskite Oxide Redox Mediators

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