Ultrathin and Conformal Depletion Layer of Core/Shell Heterojunction Enables Efficient and Stable Acidic Water Oxidation

Ru-based electrocatalysts hold great promise for developing affordable proton exchange membrane (PEM) electrolyzers. However, the harsh acidic oxidative environment of the acidic oxygen evolution reaction (OER) often causes undesirable overoxidation of Ru active sites and subsequent serious activity loss. Here, we present an ultrathin and conformal depletion layer attached to the Schottky heterojunction of core/shell RuCo/RuCoO<sub><i>x</i></sub> that not only maximizes the availability of active sites but also improves its durability and intrinsic activity for acidic OER. Operando synchrotron characterizations combined with theoretical calculations elucidate that the lattice strain and charge transfer induced by Schottky heterojunction substantially regulate the electronic structures of active sites, which modulates the OER pathway and suppresses the overoxidation of Ru species. Significantly, the closed core/shell architecture of the RuCo/RuCoO<sub><i>x</i></sub> ensures the structure integrity of the Schottky heterojunction under acidic OER conditions. As a result, the core/shell RuCo/RuCoO<sub><i>x</i></sub> Schottky heterojunction exhibits an unprecedented durability up to 250 0 h at 10 mA cm<sup>-2</sup> with an ultralow overpotential of ∼170 mV at 10 mA cm<sup>-2</sup> in 0.5 M H<sub>2</sub>SO<sub>4</sub>. The RuCo/RuCoO<sub><i>x</i></sub> catalyst also demonstrates superior durability in a proton exchange membrane (PEM) electrolyzer, showcasing the potential for practical applications.

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Publication Details

Journal
Journal of the American Chemical Society
Published
2024-09-23
DOI
https://doi.org/10.1021/jacs.4c07995
Citations
69
Primary Topic
Semiconductor materials and devices
Type
article
Field-Weighted Citation Impact
14.40

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article

Ultrathin and Conformal Depletion Layer of Core/Shell Heterojunction Enables Efficient and Stable Acidic Water Oxidation

Xiaoke Xi, Jianghua Wu, Haeseong Jang, Shuhong Jiao et al.
69 citations
Journal of the American Chemical Society
Semiconductor materials and devices
14.40
article

Ultrathin and Conformal Depletion Layer of Core/Shell Heterojunction Enables Efficient and Stable Acidic Water Oxidation

Xiaoke Xi, Jianghua Wu, Haeseong Jang, Shuhong Jiao, Donglai Zhou, Yu Deng, Ruiguo Cao, Wensheng Yan, Wanxia Li, Feng Zhu, Meng Gu, Yuchen Zhang, Min Gyu Kim, Jun Jiang, Zhanwu Lei, Huirong Li, Yan Huang, Duojie Wu, Yang Liu
article en
69 citations

Abstract

Ru-based electrocatalysts hold great promise for developing affordable proton exchange membrane (PEM) electrolyzers. However, the harsh acidic oxidative environment of the acidic oxygen evolution reaction (OER) often causes undesirable overoxidation of Ru active sites and subsequent serious activity loss. Here, we present an ultrathin and conformal depletion layer attached to the Schottky heterojunction of core/shell RuCo/RuCoO<sub><i>x</i></sub> that not only maximizes the availability of active sites but also improves its durability and intrinsic activity for acidic OER. Operando synchrotron characterizations combined with theoretical calculations elucidate that the lattice strain and charge transfer induced by Schottky heterojunction substantially regulate the electronic structures of active sites, which modulates the OER pathway and suppresses the overoxidation of Ru species. Significantly, the closed core/shell architecture of the RuCo/RuCoO<sub><i>x</i></sub> ensures the structure integrity of the Schottky heterojunction under acidic OER conditions. As a result, the core/shell RuCo/RuCoO<sub><i>x</i></sub> Schottky heterojunction exhibits an unprecedented durability up to 250 0 h at 10 mA cm<sup>-2</sup> with an ultralow overpotential of ∼170 mV at 10 mA cm<sup>-2</sup> in 0.5 M H<sub>2</sub>SO<sub>4</sub>. The RuCo/RuCoO<sub><i>x</i></sub> catalyst also demonstrates superior durability in a proton exchange membrane (PEM) electrolyzer, showcasing the potential for practical applications.

Journal of the American Chemical SocietyVol. 146(39)
Pohang University of Science and Technology (KR), University of Science and Technology of China (CN), City University of Hong Kong (HK), Hefei National Center for Physical Sciences at Nanoscale (CN), City University of Hong Kong, Shenzhen Research Institute (CN), Collaborative Innovation Center of Advanced Microstructures (CN), National Synchrotron Radiation Laboratory (CN), Pohang Accelerator Laboratory, Eastern Institute of Technology, Ningbo, Chung-Ang University (KR), Nanjing University (CN)
National Natural Science Foundation of China, Chinese Academy of Sciences, National Key Research and Development Program of China
Clean water and sanitation
Openalex Percentile: Top 1%
Semiconductor materials and devices
14.40
DOISourceOpenAlex
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