Stabilizing Highly Active Ru Sites by Suppressing Lattice Oxygen Participation in Acidic Water Oxidation

Yunzhou Wen(Fudan University), Peining Chen(University of Toronto), Lu Wang(California Institute of Technology), Shangyu Li(Fudan University), Ziyun Wang(University of Toronto), Jehad Abed(University of Toronto), Xinnan Mao(Soochow University), Yimeng Min(University of Toronto), Cao‐Thang Dinh(Queen's University), Phil De Luna(University of Toronto), Rui Huang(Fudan University), Longsheng Zhang(Fudan University), Lie Wang(California Institute of Technology), Liping Wang(California Institute of Technology), Robert J. Nielsen(California Institute of Technology), Huihui Li(University of Toronto), Tao‐Tao Zhuang(University of Toronto), Changchun Ke(Shanghai Jiao Tong University), Oleksandr Voznyy(University of Toronto), Yongfeng Hu(Canadian Light Source (Canada)), Youyong Li(Soochow University), William A. Goddard(California Institute of Technology), Bo Zhang(Fudan University), Huisheng Peng(Fudan University), Edward H. Sargent(University of Toronto)
Journal of the American Chemical Society
April 23, 2021
Cited by 540Open Access
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Abstract

In hydrogen production, the anodic oxygen evolution reaction (OER) limits the energy conversion efficiency and also impacts stability in proton-exchange membrane water electrolyzers. Widely used Ir-based catalysts suffer from insufficient activity, while more active Ru-based catalysts tend to dissolve under OER conditions. This has been associated with the participation of lattice oxygen (lattice oxygen oxidation mechanism (LOM)), which may lead to the collapse of the crystal structure and accelerate the leaching of active Ru species, leading to low operating stability. Here we develop Sr–Ru–Ir ternary oxide electrocatalysts that achieve high OER activity and stability in acidic electrolyte. The catalysts achieve an overpotential of 190 mV at 10 mA cm–2 and the overpotential remains below 225 mV following 1,500 h of operation. X-ray absorption spectroscopy and 18O isotope-labeled online mass spectroscopy studies reveal that the participation of lattice oxygen during OER was suppressed by interactions in the Ru–O–Ir local structure, offering a picture of how stability was improved. The electronic structure of active Ru sites was modulated by Sr and Ir, optimizing the binding energetics of OER oxo-intermediates.


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