Manganese-based A-site high-entropy perovskite oxide for solar thermochemical hydrogen production

Liu, Cijie; Zhang, Dawei; Li, Wei; Trindell, Jamie A.; King, Keith A.; Bishop, Sean R.; Sugar, Joshua D.; McDaniel, Anthony H.; Smith, Andrew I.; Salinas, Perla A.; Coker, Eric N.; Clauser, Arielle L.; Velayutham, Murugesan; Neuefeind, Joerg C.; Yang, Jingjing; De Santiago, Héctor A.; Ma, Liang; Wang, Yi; Wang, Qiang; Li, Wenyuan; Wang, Qingsong; Li, Qingyuan; Tian, Hanchen; Ngan Tran, Ha Ngoc; Li, Xuemei; Robinson, Brandon; Deibel, Angela M.; Collins, Gregory; Thieu, Nhat Anh; Hu, Jianli; Khramtsov, Valery V.; Luo, Jian; Liu, Xingbo

doi:10.1039/d3ta03554a

Manganese-based A-site high-entropy perovskite oxide for solar thermochemical hydrogen production

Journal Article · Sun Dec 17 23:00:00 EST 2023 · Journal of Materials Chemistry. A

DOI:https://doi.org/10.1039/d3ta03554a· OSTI ID:2317743

Liu, Cijie ^[1]; Zhang, Dawei ^[2]; ^[1]; Trindell, Jamie A. ^[3]; King, Keith A. ^[3]; Bishop, Sean R. ^[4]; Sugar, Joshua D. ^[3]; McDaniel, Anthony H. ^[3]; Smith, Andrew I. ^[4]; Salinas, Perla A. ^[4]; ^[4]; Clauser, Arielle L. ^[3]; Velayutham, Murugesan ^[1]; Neuefeind, Joerg C. ^[5]; Yang, Jingjing ^[2]; De Santiago, Héctor A. ^[1]; Ma, Liang ^[1]; Wang, Yi ^[1]; Wang, Qiang ^[1]; ^[1] more »

West Virginia Univ., Morgantown, WV (United States)
Univ. of San Diego, La Jolla, CA (United States)
Sandia National Laboratories (SNL-CA), Livermore, CA (United States)
Sandia National Laboratories (SNL-NM), Albuquerque, NM (United States)
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
Univ. of Bayreuth (Germany)

Non-stoichiometric perovskite oxides have been studied as a new family of redox oxides for solar thermochemical hydrogen (STCH) production owing to their favourable thermodynamic properties. However, conventional perovskite oxides suffer from limited phase stability and kinetic properties, and poor cyclability. Here, we report a strategy of introducing A-site multi-principal-component mixing to develop a high-entropy perovskite oxide, (La_1/6Pr_1/6Nd_1/6Gd_1/6Sr_1/6Ba_1/6)MnO₃ (LPNGSB_Mn), which shows desirable thermodynamic and kinetics properties as well as excellent phase stability and cycling durability. LPNGSB_Mn exhibits enhanced hydrogen production (~77.5 mmol mol_oxide^-1) compared to (La_2/3Sr_1/3)MnO₃ (~53.5 mmol mol_oxide^-1) in a short 1 hour redox duration and high STCH and phase stability for 50 cycles. LPNGSB_Mn possesses a moderate enthalpy of reduction (252.51–296.32 kJ (mol O)^-1), a high entropy of reduction (126.95–168.85 J (mol O)^-1 K^-1), and fast surface oxygen exchange kinetics. All A-site cations do not show observable valence changes during the reduction and oxidation processes. In conclusion, this research preliminarily explores the use of one A-site high-entropy perovskite oxide for STCH.

View Accepted Manuscript (DOE)

Research Organization:: Sandia National Laboratories (SNL-NM), Albuquerque, NM (United States); National Renewable Energy Laboratory (NREL), Golden, CO (United States); Univ. of San Diego, La Jolla, CA (United States)

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE), Office of Sustainable Transportation. Hydrogen Fuel Cell Technologies Office (HFTO); USDOE National Nuclear Security Administration (NNSA); USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF); National Science Foundation (NSF)

Grant/Contract Number:: NA0003525; AC36-08GO28308; EE0008839

OSTI ID:: 2317743

Alternate ID(s):: OSTI ID: 2482633
OSTI ID: 2281610

Report Number(s):: SAND--2024-02269J

Journal Information:: Journal of Materials Chemistry. A, Journal Name: Journal of Materials Chemistry. A Journal Issue: 7 Vol. 12; ISSN 2050-7488

Publisher:: Royal Society of ChemistryCopyright Statement

Country of Publication:: United States

Language:: English

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Manganese-based A-site high-entropy perovskite oxide for solar thermochemical hydrogen production

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