In-situ spectroscopic observation of dynamic-coupling oxygen on atomically dispersed iridium electrocatalyst for acidic water oxidation

Hui Su, Wanlin Zhou, Wu Zhou, Yuanli Li, Lirong Zheng, Hui Zhang, Meihuan Liu, Xiuxiu Zhang, Xuan Sun, Yanzhi Xu, Fengchun Hu, Jing Zhang, Tiandou Hu, Qinghua Liu () and Shiqiang Wei ()
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Hui Su: National Synchrotron Radiation Laboratory, University of Science and Technology of China
Wanlin Zhou: National Synchrotron Radiation Laboratory, University of Science and Technology of China
Wu Zhou: School of Chemistry and Chemical Engineering, Key Laboratory for Green Processing of Chemical Engineering of Xinjiang Bingtuan, Shihezi University
Yuanli Li: National Synchrotron Radiation Laboratory, University of Science and Technology of China
Lirong Zheng: Beijing Synchrotron Radiation Facility, Institute of High Energy Physics, Chinese Academy of Sciences
Hui Zhang: National Synchrotron Radiation Laboratory, University of Science and Technology of China
Meihuan Liu: National Synchrotron Radiation Laboratory, University of Science and Technology of China
Xiuxiu Zhang: National Synchrotron Radiation Laboratory, University of Science and Technology of China
Xuan Sun: National Synchrotron Radiation Laboratory, University of Science and Technology of China
Yanzhi Xu: National Synchrotron Radiation Laboratory, University of Science and Technology of China
Fengchun Hu: National Synchrotron Radiation Laboratory, University of Science and Technology of China
Jing Zhang: Beijing Synchrotron Radiation Facility, Institute of High Energy Physics, Chinese Academy of Sciences
Tiandou Hu: Beijing Synchrotron Radiation Facility, Institute of High Energy Physics, Chinese Academy of Sciences
Qinghua Liu: National Synchrotron Radiation Laboratory, University of Science and Technology of China
Shiqiang Wei: National Synchrotron Radiation Laboratory, University of Science and Technology of China

Nature Communications, 2021, vol. 12, issue 1, 1-9

Abstract: Abstract Uncovering the dynamics of active sites in the working conditions is crucial to realizing increased activity, enhanced stability and reduced cost of oxygen evolution reaction (OER) electrocatalysts in proton exchange membrane electrolytes. Herein, we identify at the atomic level potential-driven dynamic-coupling oxygen on atomically dispersed hetero-nitrogen-configured Ir sites (AD-HN-Ir) in the OER working conditions to successfully provide the atomically dispersed Ir electrocatalyst with ultrahigh electrochemical acidic OER activity. Using in-situ synchrotron radiation infrared and X-ray absorption spectroscopies, we directly observe that one oxygen atom is formed at the Ir active site with an O-hetero-Ir-N4 structure as a more electrophilic active centre in the experiment, which effectively promotes the generation of key *OOH intermediates under working potentials; this process is favourable for the dissociation of H2O over Ir active sites and resistance to over-oxidation and dissolution of the active sites. The optimal AD-HN-Ir electrocatalyst delivers a large mass activity of 2860 A gmetal−1 and a large turnover frequency of 5110 h−1 at a low overpotential of 216 mV (10 mA cm−2), 480–510 times larger than those of the commercial IrO2. More importantly, the AD-HN-Ir electrocatalyst shows no evident deactivation after continuous 100 h OER operation in an acidic medium.

Date: 2021
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DOI: 10.1038/s41467-021-26416-3

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