Nature Communications ( IF 14.7 ) Pub Date : 2023-10-13 , DOI: 10.1038/s41467-023-42221-6 Qiang Fu 1 , Lok Wing Wong 1 , Fangyuan Zheng 1 , Xiaodong Zheng 1 , Chi Shing Tsang 1 , Ka Hei Lai 1 , Wenqian Shen 1 , Thuc Hue Ly 2, 3, 4 , Qingming Deng 5 , Jiong Zhao 1, 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 NiPS3 nanosheets for alkaline hydrogen production. Using in situ electrochemical transmission electron microscopy technique, we confirmed the amorphization process occurred on the edges of NiPS3 is critical for achieving superior activity. Comprehensive characterizations and theoretical calculations reveal Ru primarily stabilized at edges of NiPS3 through in situ formed amorphous layer containing bridging S22− 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.
中文翻译:
揭示并利用原位表面非晶化增强碱性介质中的析氢反应
表面非晶化为电催化剂提供了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然缺乏实验观察和机制解释。在此,我们提出了这样的概念:通过原位重建非晶表面,金属磷三硫属化物本质上可以为碱性氢生产提供更好的催化性能。将微量 Ru (0.81 wt.%) 掺杂到 NiPS 3纳米片中用于生产碱性氢。使用原位电化学透射电子显微镜技术,我们证实 NiPS 3边缘发生的非晶化过程对于实现优异的活性至关重要。综合表征和理论计算表明,Ru通过原位形成的含有桥联S 2 2−物种的非晶层主要稳定在NiPS 3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,并表明其优化电催化剂催化活性的潜力。