Citation: Weicheng Feng, Jingcheng Yu, Yilan Yang, Yige Guo, Geng Zou, Xiaoju Liu, Zhou Chen, Kun Dong, Yuefeng Song, Guoxiong Wang, Xinhe Bao. Regulating the High Entropy Component of Double Perovskite for High-Temperature Oxygen Evolution Reaction[J]. Acta Physico-Chimica Sinica, ;2024, 40(6): 230601. doi: 10.3866/PKU.WHXB202306013 shu

Regulating the High Entropy Component of Double Perovskite for High-Temperature Oxygen Evolution Reaction

Weicheng Feng ^{1, 2, †} ,
Jingcheng Yu ^{1, 2, †} ,
Yilan Yang ³ ,
Yige Guo ^{1, 2} ,
Geng Zou ^{1, 2} ,
Xiaoju Liu ⁴ ,
Zhou Chen ⁵ ,
Kun Dong ⁶ ,
Yuefeng Song ^1,, ,
Guoxiong Wang ^1,, ,
Xinhe Bao ¹

1.
State Key Laboratory of Catalysis, Dalian National Laboratory for Clean Energy, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, Liaoning Province, China
2.
College of Energy, University of Chinese Academy of Sciences, Beijing 100049, China
3.
School of Environmental and Chemical Engineering, Dalian Jiaotong University, Dalian 116028, Liaoning Province, China
4.
School of Chemistry and Chemical Engineering, Yulin University, Yulin 719100, Shannxi Province, China
5.
College of Materials, Xiamen University, Xiamen 361005, Fujian Province, China
6.
Beijing Key Laboratory of Ionic Liquids Clean Process, State Key Laboratory of Multiphase Complex Systems, Institute of Process Engineering, Chinese Academy of Sciences, Beijing 100190, China

Corresponding author: Yuefeng Song, Guoxiong Wang,
Received Date: 5 June 2023
Revised Date: 31 July 2023
Accepted Date: 31 July 2023
Available Online: 10 August 2023
Fund Project: the National Key R & D Program of China 2021YFA1502400the National Natural Science Foundation of China 22272176the National Natural Science Foundation of China 22002166the National Natural Science Foundation of China 22125205the National Natural Science Foundation of China 22072146the National Natural Science Foundation of China 22002158the DNL Cooperation Fund, CAS DNL202007the Joint Fund of the Yulin University and the Dalian National Laboratory for Clean Energy YLU-DNL Fund 2022008the CAS Youth Innovation Promotion Y201938

Solid oxide electrolysis cells (SOECs) could convert CO₂ to CO powered by clean electricity with low overpotential, high Faradaic efficiency, and high current density. Since the performance of SOEC is affected by sluggish oxygen evolution reaction (OER) kinetics at the anodes, the modification of anode materials is crucial for the further application of SOEC. Perovskites with high configurational entropy exhibit high catalytic activity in many reactions, but are rarely reported in SOECs. Herein, two kinds of high entropy perovskites (HEPs), with formulas of (Pr_0.2La_0.2Sm_0.2Nd_0.2Gd_0.2)BaCo₂O_6−δ (A-HEP) and Pr(Ba_0.2Sr_0.2Ca_0.2Na_0.2K_0.2) Co₂O_6−δ (A′-HEP), are synthesized by doping different rare earth metal, and alkaline metal or alkaline earth metal ions into A-site and A′-site of the double perovskites. Rietveld refinement of X-ray diffraction patterns and elemental maps of scanning electron microscope images confirm the successful synthesis of the two samples. The tetragonal double perovskite structure of A-HEP and the transformation to orthorhombic structure of A′-HEP due to the difference in average atomic radii and oxidation states of the doped ions are also detected. Co 2p X-ray photoelectron spectroscopy (XPS) and O K-edge X-ray absorption spectroscopy reveal that the average oxidation state of Co is lifted from +3.23 in Aʹ-HEP to +3.39 in A-HEP, and the hybridization of Co 2p and O 1s orbitals is also enhanced in A-HEP, which increase the electron transfer pathway and reduce the transfer barrier. Therefore, the electrical conductivity of A-HEP at 800 ℃ is higher than that of Aʹ-HEP. Moreover, the increased absorption oxygen species concentration of A-HEP in O 1s XPS and O₂-temperature programmed desorption results indicates more surface oxygen vacancies, thus increasing active sites for the anodic OER. Consequently, the anodic polarization resistances related to oxygen transportation, electron transfer and surface reaction processes are decreased remarkably in A-HEP, resulting in a high current density of 1.76 A∙cm⁻² at 800 ℃ and a stability of 200 h. This work presents a new method for designing high-performance HEPs as SOEC anode materials.
- Solid oxide electrolysis cell,
- High entropy perovskite,
- Oxygen evolution reaction,
- Oxygen vacancy,
- Electron transfer
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