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

IF 14.7 1区综合性期刊 Q1 MULTIDISCIPLINARY SCIENCES

Nature Communications Pub Date : 2025-07-12 DOI:10.1038/s41467-025-61871-2

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

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Abstract

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_s-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.

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生物启发的硫氧桥优化界面水结构，增强氢氧化和进化反应

揭示水在电极-溶液界面的动态结构对于各种电催化过程至关重要，其中水作为质子和电子源。然而，精确控制复杂界面上水的状态仍然具有挑战性。受天然酶中金属蛋白的启发，我们在此证明了Co和Ru位点之间的亲水亚氧桥接（Cos-SO-Ru）通过有利的氢键网络优化了界面水结构，促进了氢的氧化和进化反应。机理研究表明，立体硫氧桥通过排斥电极表面的阳离子，增强了氢键网络的连通性，促进了质子转移过程。此外，Co给电子位点降低了Ru的表面亲氧性，优化了羟基的吸附-解吸行为，控制了及时刷新的Ru位点，从而提高了催化性能。这种受生物启发的活性位点为精确设计界面水结构以改善电催化提供了不同的途径。

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来源期刊

Nature Communications Biological Science Disciplines-

CiteScore

24.90

自引率

2.40%

发文量

6928

审稿时长

3.7 months

期刊介绍： Nature Communications, an open-access journal, publishes high-quality research spanning all areas of the natural sciences. Papers featured in the journal showcase significant advances relevant to specialists in each respective field. With a 2-year impact factor of 16.6 (2022) and a median time of 8 days from submission to the first editorial decision, Nature Communications is committed to rapid dissemination of research findings. As a multidisciplinary journal, it welcomes contributions from biological, health, physical, chemical, Earth, social, mathematical, applied, and engineering sciences, aiming to highlight important breakthroughs within each domain.