Fu Qiang, Wong Lok Wing, Zheng Fangyuan, Zheng Xiaodong, Tsang Chi Shing, Lai Ka Hei, Shen Wenqian, Ly Thuc Hue, Deng Qingming, Zhao Jiong
Department of Applied Physics, The Hong Kong Polytechnic University, Kowloon, China.
Department of Chemistry and Center of Super-Diamond & Advanced Films (COSDAF), City University of Hong Kong, Kowloon, China.
Nat Commun. 2023 Oct 13;14(1):6462. doi: 10.1038/s41467-023-42221-6.
Surface amorphization provides electrocatalysts with more active sites and flexibility. However, there is still a lack of experimental observations and mechanistic explanations for the in situ amorphization process and its crucial role. Herein, we propose the concept that by in situ reconstructed amorphous surface, metal phosphorus trichalcogenides could intrinsically offer better catalytic performance for the alkaline hydrogen production. Trace Ru (0.81 wt.%) is doped into NiPS nanosheets for alkaline hydrogen production. Using in situ electrochemical transmission electron microscopy technique, we confirmed the amorphization process occurred on the edges of NiPS is critical for achieving superior activity. Comprehensive characterizations and theoretical calculations reveal Ru primarily stabilized at edges of NiPS through in situ formed amorphous layer containing bridging S species, which can effectively reduce the reaction energy barrier. This work emphasizes the critical role of in situ formed active layer and suggests its potential for optimizing catalytic activities of electrocatalysts.
表面非晶化赋予电催化剂更多的活性位点和灵活性。然而，对于原位非晶化过程及其关键作用，仍缺乏实验观察和机理解释。在此，我们提出了一个概念，即通过原位重构非晶表面，金属三硫属磷化物能够本质上为碱性析氢提供更好的催化性能。将痕量Ru（0.81 wt.%）掺杂到NiPS纳米片中用于碱性析氢。利用原位电化学透射电子显微镜技术，我们证实了在NiPS边缘发生的非晶化过程对于实现优异活性至关重要。综合表征和理论计算表明，Ru主要通过原位形成的含有桥连S物种的非晶层稳定在NiPS的边缘，这可以有效降低反应能垒。这项工作强调了原位形成的活性层的关键作用，并表明了其在优化电催化剂催化活性方面的潜力。
