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

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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:
Manganese-based A-site high-entropy perovskite oxide for solar thermochemical hydrogen production.
In: Journal of Materials Chemistry A. Bd. 12 (2024) Heft 7 . - S. 3910-3922.
ISSN 2050-7496
DOI: https://doi.org/10.1039/D3TA03554A

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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, (La1/6Pr1/6Nd1/6Gd1/6Sr1/6Ba1/6)MnO3 (LPNGSBMn), which shows desirable thermodynamic and kinetics properties as well as excellent phase stability and cycling durability. LPNGSBMn exhibits enhanced hydrogen production (∼77.5 mmol moloxide−1) compared to (La2/3Sr1/3)MnO3 (∼53.5 mmol moloxide−1) in a short 1 hour redox duration and high STCH and phase stability for 50 cycles. LPNGSBMn 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.