Atomic-Scale Observation of Bimetallic Au-CuOx Nanoparticles and Their Interfaces for Activation of CO Molecules

双金属片 材料科学 纳米团簇 成核 纳米颗粒 催化作用 扫描透射电子显微镜 原子单位 金属 吸附 胶体金 化学工程 纳米技术 透射电子显微镜 分子 物理化学 化学 冶金 工程类 物理 有机化学 量子力学 生物化学
作者
Jingjie Luo,Yuefeng Liu,Liyun Zhang,Yujing Ren,Shu Miao,Bingsen Zhang,Dang Sheng Su,Changhai Liang
出处
期刊:ACS Applied Materials & Interfaces [American Chemical Society]
卷期号:11 (38): 35468-35478 被引量:24
标识
DOI:10.1021/acsami.9b12017
摘要

Supported gold nanoparticles with sizes below 5 nm display attractive catalytic activities for heterogeneous reactions, particularly those promoted by secondary metal (e.g., Cu) because of the well-defined synergy between metal compositions. However, the specific atomic structure at interfaces is less interpreted systematically. In this work, various bimetallic Au-CuOx catalysts with specific surface structures were synthesized and explored by aberration-corrected scanning transmission electron microscopy (AC-STEM), temperature-programmed experiments and in situ DRIFT experiments. Results suggest that the atomic structure and interfaces between gold and CuOx are determined by the nucleation behaviors of the nanoparticles and result in subsequently the distinctive ability for CO activation. Bimetallic CuO*/Au sample formatted by gold particles surrounded with CuOx nanoclusters have rough surface with prominently exposed low-coordinated Au step defects. Whereas the bimetallic Au@CuO sample formatted by copper precursor in the presence of gold nanoparticles have core-shell structure with relatively smooth surface. The former structure of CuO*/Au displays much accelerated properties for CO adsorption and activation with 90% CO converted to CO2 at 90 °C and nice stability with time on stream. The results clearly determine from atomic scale the significance of exposed gold step sites and intrinsic formation of defected surface by different nucleation. The above properties are directly responsible for the induced variation in chemical composition and the catalytic activity.
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