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一氧化碳加氢反应中相邻铂单体之间的协同相互作用。

Synergetic interaction between neighbouring platinum monomers in CO hydrogenation.

作者信息

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

机构信息

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.

出版信息

Nat Nanotechnol. 2018 May;13(5):411-417. doi: 10.1038/s41565-018-0089-z. Epub 2018 Mar 19.


DOI:10.1038/s41565-018-0089-z
PMID:29556007
Abstract

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.

摘要

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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Precis Chem. 2023-5-26

[2]
In Situ High-Temperature Reaction-Induced Local Structural Dynamic Evolution of Single-Atom Pt on Oxide Support.

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[3]
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[4]
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Angew Chem Int Ed Engl. 2025-8-4

[5]
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Nano Lett. 2025-6-4

[6]
Soft nanoforest of metal single atoms for free diffusion catalysis.

Sci Adv. 2025-1-17

[7]
Efficient amine-assisted CO hydrogenation to methanol co-catalyzed by metallic and oxidized sites within ruthenium clusters.

Nat Commun. 2025-1-11

[8]
General synthesis of neighboring dual-atomic sites with a specific pre-designed distance via an interfacial-fixing strategy.

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[9]
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[10]
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