电场偏压诱导的1T'-MoS₂上单核与异核双原子催化剂的可逆构型
Electric bias-induced reversible configuration of single and heteronuclear dual-atom catalysts on 1T'-MoS.
作者信息
Wu Jianhua, Chen Zhongxin, Yang Ke, Zhou Xin, Li Huizhi, Wang Zhiyong, Su Mengyao, Zhang Rongrong, Wang Tie, Hu Qikun, Yan Ning, Liu Cuibo, Zhang Bin, Yang Ming, Xi Shibo, Loh Kian Ping
机构信息
Department of Chemistry, National University of Singapore, Singapore, Singapore.
School of Science and Engineering, The Chinese University of Hong Kong, Shenzhen, China.
出版信息
Nat Nanotechnol. 2025 May 19. doi: 10.1038/s41565-025-01934-z.
The development of substrates capable of anchoring single-atom catalysts (SACs) while enabling their dynamic reconfiguration into heteronuclear dual-atom catalysts (DACs) holds considerable promise for electrochemical synthesis, yet remains underexplored. Here we show that electrochemical desulfurization of MoS generates vacancy-rich 1T' domains, which support high loadings of Cu (7.9 wt%) and Pt (6.7 wt%) SACs that are well-positioned for dynamic sintering to form DACs. Operando X-ray absorption spectroscopy and density functional theory calculations reveal a voltage-driven, reversible transformation between individual Pt/Cu SACs and Cu-Pt DAC configurations during hydrogen evolution reaction potentials. The electric-field-induced Cu-Pt DACs exhibit superior performance in the selective hydrogenation of alkynes compared with their monometallic SAC counterparts. This work underscores vacancy-enriched 1T'-MoS as a versatile platform for high-density SAC deposition, enabling on-demand structural reconfiguration and paving the way for tailored catalyst design in electrosynthesis.
能够锚定单原子催化剂（SAC）并使其动态重构为异核双原子催化剂（DAC）的基底的开发，对电化学合成具有巨大潜力，但仍未得到充分探索。在此，我们表明，对MoS进行电化学脱硫会产生富含空位的1T'域，这些域可负载高含量的Cu（7.9 wt%）和Pt（6.7 wt%）单原子催化剂，这些单原子催化剂为动态烧结形成双原子催化剂提供了良好的条件。原位X射线吸收光谱和密度泛函理论计算表明，在析氢反应电位下，单个Pt/Cu单原子催化剂与Cu-Pt双原子催化剂构型之间存在电压驱动的可逆转变。与单金属单原子催化剂相比，电场诱导的Cu-Pt双原子催化剂在炔烃选择性加氢反应中表现出优异的性能。这项工作强调了富含空位的1T'-MoS作为高密度单原子催化剂沉积的通用平台，能够按需进行结构重构，并为电合成中定制催化剂设计铺平了道路。
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