Activating lattice oxygen in high-entropy LDH for robust and durable water oxidation

Fangqing Wang; Peichao Zou; Yangyang Zhang; Wenli Pan; Ying Li; Limin Liang; Cong Chen; Hui Liu; Shijian Zheng

doi:10.1038/s41467-023-41706-8

Activating lattice oxygen in high-entropy LDH for robust and durable water oxidation

Nat Commun. 2023 Sep 27;14(1):6019. doi: 10.1038/s41467-023-41706-8.

Authors

Fangqing Wang^{1

2}, Peichao Zou³, Yangyang Zhang², Wenli Pan⁴, Ying Li^{1

2}, Limin Liang², Cong Chen², Hui Liu^{5

6}, Shijian Zheng^{7

8}

Affiliations

¹ Key Laboratory of Special Functional Materials for Ecological Environment and Information (Ministry of Education), Hebei University of Technology, Tianjin, 300130, PR China.
² School of Material Science and Engineering, Hebei University of Technology, Tianjin, 300130, PR China.
³ Department of Physics and Astronomy, University of California, Irvine, CA, 92697, USA.
⁴ Graduate School of Human and Environmental Studies, Kyoto University, Yoshida-nihonmatsu-cho, Sakyo, Kyoto, 606-8501, Japan.
⁵ Key Laboratory of Special Functional Materials for Ecological Environment and Information (Ministry of Education), Hebei University of Technology, Tianjin, 300130, PR China. liuhui2013@hebut.edu.cn.
⁶ School of Material Science and Engineering, Hebei University of Technology, Tianjin, 300130, PR China. liuhui2013@hebut.edu.cn.
⁷ Key Laboratory of Special Functional Materials for Ecological Environment and Information (Ministry of Education), Hebei University of Technology, Tianjin, 300130, PR China. sjzheng@hebut.edu.cn.
⁸ School of Material Science and Engineering, Hebei University of Technology, Tianjin, 300130, PR China. sjzheng@hebut.edu.cn.

Abstract

The oxygen evolution reaction is known to be a kinetic bottleneck for water splitting. Triggering the lattice oxygen oxidation mechanism (LOM) can break the theoretical limit of the conventional adsorbate evolution mechanism and enhance the oxygen evolution reaction kinetics, yet the unsatisfied stability remains a grand challenge. Here, we report a high-entropy MnFeCoNiCu layered double hydroxide decorated with Au single atoms and O vacancies (Au_SA-MnFeCoNiCu LDH), which not only displays a low overpotential of 213 mV at 10 mA cm^-2 and high mass activity of 732.925 A g^-1 at 250 mV overpotential in 1.0 M KOH, but also delivers good stability with 700 h of continuous operation at ~100 mA cm^-2. Combining the advanced spectroscopic techniques and density functional theory calculations, it is demonstrated that the synergistic interaction between the incorporated Au single atoms and O vacancies leads to an upshift in the O 2p band and weakens the metal-O bond, thus triggering the LOM, reducing the energy barrier, and boosting the intrinsic activity.

Abstract

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