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

被引:24
作者
Luo, Jingjie [1 ,2 ]
Liu, Yuefeng [3 ]
Zhang, Liyun [4 ,5 ]
Ren, Yujing [3 ]
Miao, Shu [3 ]
Zhang, Bingsen [4 ]
Su, Dang Sheng [3 ]
Liang, Changhai [1 ,2 ]
机构
[1] Dalian Univ Technol, Sch Chem Engn, State Key Lab Fine Chem, Panjin Campus, Panjin 124221, Peoples R China
[2] Dalian Univ Technol, Sch Chem Engn, Lab Adv Mat & Catalyt Engn AMCE, Panjin Campus, Panjin 124221, Peoples R China
[3] Chinese Acad Sci, Dalian Inst Chem Phys, Dalian Natl Lab Clean Energy DNL, 457 Zhongshan Rd, Dalian 116023, Peoples R China
[4] Chinese Acad Sci, Inst Met Res, Shenyang Natl Lab Mat Sci SYNL, 72 Wenhua Rd, Shenyang 110016, Liaoning, Peoples R China
[5] Qufu Normal Univ, Dept Chem Engn, Qufu 273165, Peoples R China
基金
中国国家自然科学基金;
关键词
Au catalysis; Au-Cu bimetallic particles; defect-enriched surface; step sites; CO activation; CATALYTIC-OXIDATION; GOLD NANOPARTICLES; METAL-OXIDES; PROMOTION; CERIA; PHOTOPRODUCTION; NANOCRYSTALS; ENHANCEMENT; CONVERSION; STRATEGY;
D O I
10.1021/acsami.9b12017
中图分类号
TB3 [工程材料学];
学科分类号
0805 ; 080502 ;
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 a 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 degrees 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.
引用
收藏
页码:35468 / 35478
页数:11
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