<p>Uncovering the dynamic structures of water at the electrode-solution interface is crucial for various electrocatalysis processes, where water acts as a proton and electron source. However, precisely controlling the state of water on complex interfaces remains challenging. Inspired by the metalloproteins in natural enzymes, we herein demonstrate that the hydrophilic sulfo-oxygen bridging between Co and Ru sites (Co<sub>s</sub>-SO-Ru) optimizes interfacial water structure via a favorable hydrogen-bond network, promoting hydrogen oxidation and evolution reactions. Mechanistic studies reveal that the stereoscopic sulfo-oxygen bridges enhance the connectivity of hydrogen-bond network to promote the proton transfer process via repelling cations from the electrode surface. Furthermore, electron donating Co sites reduce the surface oxophilicity of Ru to optimize the adsorption-desorption behaviors of hydroxyl, governing the timely refreshed Ru sites to enhance catalytic performances. Such bioinspired active sites offer a different pathway for the precise design of interfacial water structure to improve electrocatalysis.</p>

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Bioinspired Sulfo oxygen bridges optimize interfacial water structure for enhanced hydrogen oxidation and evolution reactions

  • Chengdong Yang,
  • Yun Gao,
  • Zhengyu Xing,
  • Xinxin Shu,
  • Zechao Zhuang,
  • Yueqing Wang,
  • Yijuan Zheng,
  • Shuang Li,
  • Chong Cheng,
  • Dingsheng Wang,
  • Jintao Zhang

摘要

Uncovering the dynamic structures of water at the electrode-solution interface is crucial for various electrocatalysis processes, where water acts as a proton and electron source. However, precisely controlling the state of water on complex interfaces remains challenging. Inspired by the metalloproteins in natural enzymes, we herein demonstrate that the hydrophilic sulfo-oxygen bridging between Co and Ru sites (Cos-SO-Ru) optimizes interfacial water structure via a favorable hydrogen-bond network, promoting hydrogen oxidation and evolution reactions. Mechanistic studies reveal that the stereoscopic sulfo-oxygen bridges enhance the connectivity of hydrogen-bond network to promote the proton transfer process via repelling cations from the electrode surface. Furthermore, electron donating Co sites reduce the surface oxophilicity of Ru to optimize the adsorption-desorption behaviors of hydroxyl, governing the timely refreshed Ru sites to enhance catalytic performances. Such bioinspired active sites offer a different pathway for the precise design of interfacial water structure to improve electrocatalysis.