Li Hongliang, Wang Liangbing, Dai Yizhou, Pu Zhengtian, Lao Zhuohan, Chen Yawei, Wang Menglin, Zheng Xusheng, Zhu Junfa, Zhang Wenhua, Si Rui, Ma Chao, Zeng Jie
Hefei National Laboratory for Physical Sciences at the Microscale, Key Laboratory of Strongly-Coupled Quantum Matter Physics of Chinese Academy of Sciences, National Synchrotron Radiation Laboratory, Department of Chemical Physics, University of Science and Technology of China, Hefei, China.
Shanghai Synchrotron Radiation Facility, Shanghai Institute of Applied Physics, Chinese Academy of Sciences, Shanghai, China.
Nat Nanotechnol. 2018 May;13(5):411-417. doi: 10.1038/s41565-018-0089-z. Epub 2018 Mar 19.
Exploring the interaction between two neighbouring monomers has great potential to significantly raise the performance and deepen the mechanistic understanding of heterogeneous catalysis. Herein, we demonstrate that the synergetic interaction between neighbouring Pt monomers on MoS greatly enhanced the CO hydrogenation catalytic activity and reduced the activation energy relative to isolated monomers. Neighbouring Pt monomers were achieved by increasing the Pt mass loading up to 7.5% while maintaining the atomic dispersion of Pt. Mechanistic studies reveal that neighbouring Pt monomers not only worked in synergy to vary the reaction barrier, but also underwent distinct reaction paths compared with isolated monomers. Isolated Pt monomers favour the conversion of CO into methanol without the formation of formic acid, whereas CO is hydrogenated stepwise into formic acid and methanol for neighbouring Pt monomers. The discovery of the synergetic interaction between neighbouring monomers may create a new path for manipulating catalytic properties.
探索两个相邻单体之间的相互作用对于显著提高多相催化的性能和深化其机理理解具有巨大潜力。在此,我们证明了MoS上相邻Pt单体之间的协同相互作用相对于孤立单体极大地增强了CO加氢催化活性并降低了活化能。通过将Pt质量负载增加至7.5%同时保持Pt的原子分散性来实现相邻Pt单体。机理研究表明,相邻Pt单体不仅协同作用以改变反应势垒,而且与孤立单体相比经历了不同的反应路径。孤立的Pt单体有利于CO转化为甲醇而不形成甲酸,而对于相邻Pt单体,CO则逐步加氢生成甲酸和甲醇。相邻单体之间协同相互作用的发现可能为调控催化性能开辟一条新途径。
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