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arXiv 2603.08299cond-mat.mtrl-sci
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有机液体-固体界面中金物种的原子分辨率成像

Atomic-resolution imaging of gold species at organic liquid-solid interfaces

University of Manchester(曼彻斯特大学);National Graphene Institute, University of Manchester(曼彻斯特大学国家石墨烯研究所);Diamond Light Source(英国钻石光源实验室);Max Planck−Cardiff Centre on the Fundamentals of Heterogeneous Catalysis FUNCAT, Cardiff Catalysis Institute, School of Chemistry, Cardiff University(卡迪夫大学化学学院卡迪夫催化研究所马克斯·普朗克-卡迪夫异相催化基础中心);Cardiff Catalysis Institute, School of Chemistry, Cardiff University(卡迪夫大学化学学院卡迪夫催化研究所);School of Mathematical and Physical Sciences, University of Sheffield(谢菲尔德大学数理科学学院);University of Oxford(牛津大学);Henry Royce Institute for Advanced Materials, University of Manchester(曼彻斯特大学亨利·罗伊先进材料研究所)
Sam Sullivan-Allsop, Nick Clark, Wendong Wang, Rongsheng Cai, William Thornley, David G. Hopkinson, James G. McHugh, Ben Davies, Samuel Pattisson, Nicholas F. D… 展开作者

Sam Sullivan-Allsop, Nick Clark, Wendong Wang, Rongsheng Cai, William Thornley, David G. Hopkinson, James G. McHugh, Ben Davies, Samuel Pattisson, Nicholas F. Dummer, Rui Zhang, Matthew Lindley, Gareth Tainton, Jack Harrison, Hugo De Latour, Joseph Parker, Joshua Swindell, Eli G. Castanon, Amy Carl, David J. Lewis, Natalia Martsinovich, Christopher S. Allen, Mohsen Danaie, Andrew J. Logsdail, Vladimir Falko, Graham J. Hutchings, Alex Summerfield, Roman Gorbachev, Sarah J. Haigh

AI总结:

通过原位电子显微镜与人工智能分析,研究有机液体-固体界面中金原子的动力学行为,揭示其与溶剂和基底晶格的相互作用,为催化剂设计提供理论依据。

摘要:

理解原子尺度的固-液界面对于改进异相催化剂、电极和膜的性能至关重要。本文结合独特的样品设计、原位电子显微镜成像和人工智能分析,实现了对界面原子行为的定量理解的突破。我们创建了首个含有机溶剂的石墨烯液体细胞,并用于追踪石墨烯表面浸入乙酮和环己酮中的超过106个金原子和簇。我们揭示了金原子单体、双体、三体和簇的动态相关行为,其受彼此相互作用、溶剂性质和基底原子晶格的强烈影响,与理论计算结果一致。我们利用这些结果解释了向工业重要反应乙炔氯化反应的催化活性差异。这种探索原子尺度化学的新能力可能促进未来催化剂、膜和电极的理性设计,以提高功能性能。

英文摘要:

Understanding solid-liquid interfaces at the atomic-scale is key to improved performance of heterogeneous catalysts, electrodes and membranes. Here we combine unique specimen design, record atomic resolution in situ electron microscopy, and artificial intelligence-enabled analysis to achieve a step change in quantitative understanding of interfacial atomic behaviour. We create the first graphene liquid cells with organic solvents and employ them to track over 106 gold adatoms and clusters at a graphene surface immersed in acetone and cyclohexanone. We reveal dynamic correlated behaviour of gold adatom monomers, dimers, trimers and clusters, strongly influenced by each other, the solvent properties, and the atomic lattice of the substrate, in good agreement with theoretical calculations. We use the results to interpret differences in catalytic activity towards the industrially important acetylene hydrochlorination reaction. This new capability for exploration of atomic scale chemistry could enable rational design of future catalysts, membranes and electrodes with improved functionality.

机构、总结、中文摘要均由AI分析而来,可能存在错误,请以论文正文为准。

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