Tuning proton-coupled electron transfer by crystal orientation for efficient water oxidization on double perovskite oxides

Yunmin Zhu, Zuyun He, YongMan Choi (), Huijun Chen, Xiaobao Li, Bote Zhao, Yi Yu, Hui Zhang, Kelsey A. Stoerzinger, Zhenxing Feng, Yan Chen () and Meilin Liu ()
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Yunmin Zhu: South China University of Technology
Zuyun He: South China University of Technology
YongMan Choi: National Chiao Tung University
Huijun Chen: South China University of Technology
Xiaobao Li: State Key Laboratory of Functional Materials for Informatics, Shanghai Institute of Microsystem and Information Technology, Chinese Academy of Sciences
Bote Zhao: Materials Science and Engineering, Georgia Institute of Technology
Yi Yu: ShanghaiTech University
Hui Zhang: State Key Laboratory of Functional Materials for Informatics, Shanghai Institute of Microsystem and Information Technology, Chinese Academy of Sciences
Kelsey A. Stoerzinger: Oregon State University
Zhenxing Feng: Oregon State University
Yan Chen: South China University of Technology
Meilin Liu: Materials Science and Engineering, Georgia Institute of Technology

Nature Communications, 2020, vol. 11, issue 1, 1-10

Abstract: Abstract Developing highly efficient and cost-effective oxygen evolution reaction (OER) electrocatalysts is critical for many energy devices. While regulating the proton-coupled electron transfer (PCET) process via introducing additive into the system has been reported effective in promoting OER activity, controlling the PCET process by tuning the intrinsic material properties remains a challenging task. In this work, we take double perovskite oxide PrBa0.5Sr0.5Co1.5Fe0.5O5+δ (PBSCF) as a model system to demonstrate enhancing OER activity through the promotion of PCET by tuning the crystal orientation and correlated proton diffusion. OER kinetics on PBSCF thin films with (100), (110), and (111) orientation, deposited on single crystal LaAlO3 substrates, were investigated using electrochemical measurements, density functional theory (DFT) calculations, and synchrotron-based near ambient X-ray photoelectron spectroscopy. The results clearly show that the OER activity and the ease of deprotonation depend on orientation and follow the order of (100) > (110) > (111). Correlated with OER activity, proton diffusion is found to be the fastest in the (100) film, followed by (110) and (111) films. Our results point out a way of boosting PCET and OER activity, which can also be successfully applied to a wide range of crucial applications in green energy and environment.

Date: 2020
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DOI: 10.1038/s41467-020-17657-9

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