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理解并利用钌 - 铟合金中的纳米级不混溶性用于选择性CO加氢反应

Understanding and Harnessing Nanoscale Immiscibility in Ru-In Alloys for Selective CO Hydrogenation.

作者信息

Zhou Chengshuang, Liccardo Gennaro, Hoffman Adam S, Oh Jinwon, Holmes Sarah E, Vailionis Arturas, Bare Simon R, Cargnello Matteo

机构信息

Department of Chemical Engineering and SUNCAT Center for Interface Science and Catalysis, Stanford University, Stanford, California 94305, United States.

SSRL, SLAC National Accelerator Laboratory, Menlo Park, California 94025, United States.

出版信息

J Am Chem Soc. 2024 Jul 24;146(29):19986-19997. doi: 10.1021/jacs.4c03652. Epub 2024 Jul 10.

DOI:10.1021/jacs.4c03652
PMID:38985019
Abstract

Bimetallic alloys made from immiscible elements are characterized by their tendency to segregate on the macroscopic scale, but their behavior is known to change at the nanoscale. Here, we demonstrate that in the Ru-In system, In atoms preferentially decorate the surface of 6 nm Ru nanoparticles, forming Ru-In superficial immiscible alloys. This surface decoration dramatically affects the catalytic performance of the system, even at small atomic fractions of In added to Ru. The interfaces between Ru and In enabled unexplored methanol productivity from CO hydrogenation, which outperformed not only the individual constituents but also ordered RuIn intermetallic alloys. Our work highlights that the formation of superficial immiscible alloys could offer new insights into the understanding and design of heterogeneous catalysts.

摘要

由不互溶元素制成的双金属合金的特点是在宏观尺度上有偏析倾向,但已知它们在纳米尺度上行为会发生变化。在此,我们证明在钌 - 铟体系中,铟原子优先修饰6纳米钌纳米颗粒的表面,形成钌 - 铟表面不互溶合金。即使向钌中添加少量原子分数的铟,这种表面修饰也会显著影响该体系的催化性能。钌和铟之间的界面实现了通过一氧化碳加氢产生未被探索过的甲醇生产率,这不仅优于各单个组分,还优于有序的钌铟金属间化合物合金。我们的工作突出表明,表面不互溶合金的形成可为理解和设计多相催化剂提供新的见解。

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