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

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

doi:10.1039/D3TA03554A

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

Cijie Liu,‡^a Dawei Zhang,‡^b Wei Li,

*^a Jamie A. Trindell,^c Keith A. King,^c Sean R. Bishop,^d Joshua D. Sugar,^c Anthony H. McDaniel,^c Andrew I. Smith,^d Perla A. Salinas,^d Eric N. Coker,

^d Arielle L. Clauser,^c Murugesan Velayutham,^ef Joerg C. Neuefeind,^g Jingjing Yang,^b Héctor A. De Santiago,^a Liang Ma,^a Yi Wang,^a Qiang Wang,^h Wenyuan Li,

ⁱ Qingsong Wang,

^j Qingyuan Li,^a Hanchen Tian,^a Ha Ngoc Ngan Tran,ⁱ Xuemei Li,ⁱ Brandon Robinson,ⁱ Angela M. Deibel,

^a Gregory Collins,^a Nhat Anh Thieu,^a Jianli Hu,ⁱ Valery V. Khramtsov,

^ef Jian Luo

*^bk and Xingbo Liu

*^a

Author affiliations

* Corresponding authors

^a Department of Mechanical and Aerospace Engineering, Benjamin M. Statler College of Engineering and Mineral Resources, West Virginia University, Morgantown, WV 26506, USA
E-mail: wei.li@mail.wvu.edu, xingbo.liu@mail.wvu.edu

^b Program in Materials Science and Engineering, University of California San Diego, La Jolla, CA 92093, USA

^c Sandia National Laboratories, Livermore, CA 94551, USA

^d Sandia National Laboratories, Albuquerque, NM 87123, USA

^e In Vivo Multifunctional Magnetic Resonance Center, Robert C. Byrd Health Sciences Center, West Virginia University, Morgantown, WV 26506, USA

^f Department of Biochemistry and Molecular Medicine, School of Medicine, West Virginia University, Morgantown, WV 26506, USA

^g Chemical and Engineering Materials Division, Oak Ridge National Laboratory, Oak Ridge, TN 37831, USA

^h Shared Research Facilities, West Virginia University, Morgantown, WV 26506, USA

ⁱ Department of Chemical and Biomedical Engineering, Benjamin M. Statler College of Engineering and Mineral Resources, West Virginia University, Morgantown, WV 26506, USA

^j Department of Chemistry, Bavarian Center for Battery Technology (BayBatt), University of Bayreuth, Universitätsstrasse 30, Bayreuth, Germany

^k Department of Nano and Chemical Engineering, University of California San Diego, La Jolla, CA 92093, USA
E-mail: jluo@alum.mit.edu

Abstract

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. This research preliminarily explores the use of one A-site high-entropy perovskite oxide for STCH.

This article is part of the themed collection: Journal of Materials Chemistry A HOT Papers

Journal of Materials Chemistry A

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

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