` Site-Resolved Cu2O Catalysis in the Oxidation of CO

被引:91
作者
Zhang, Zhenhua [1 ,2 ]
Wu, Hong [1 ,2 ]
Yu, Zongyou [1 ,2 ]
Song, Rui [1 ,2 ]
Qian, Kun [1 ,2 ]
Chen, Xuanye [1 ,2 ]
Tian, Jie [3 ]
Zhang, Wenhua [1 ,2 ,4 ]
Huang, Weixin [1 ,2 ]
机构
[1] Univ Sci & Technol China, Hefei Natl Lab Phys Sci Microscale, CAS Key Lab Mat Energy Convers,Anhui Higher Educ, Key Lab Surface & Interface Chem & Energy Catalys, Hefei 230026, Anhui, Peoples R China
[2] Univ Sci & Technol China, Dept Chem Phys, Hefei 230026, Anhui, Peoples R China
[3] Univ Sci & Technol China, Engn & Mat Sci Expt Ctr, Hefei 230026, Anhui, Peoples R China
[4] Univ Sci & Technol China, Dept Mat Sci & Engn, Jinzhai Rd 96, Hefei 230026, Anhui, Peoples R China
基金
中国国家自然科学基金;
关键词
catalytic mechanisms; CO oxidation; Cu2O nanocrystals; edge sites; face sites; NANOCRYSTALS; SELECTIVITY; ORIGIN; SHAPE;
D O I
10.1002/anie.201814258
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
The identification of the contribution of different surface sites to the catalytic activity of a catalyst nanoparticle is one of the most challenging issues in the fundamental studies of heterogeneous catalysis. We herein demonstrate an effective strategy of using a series of uniform cubic Cu2O nanocrystals with different sizes to identify the intrinsic activity and contributions of face and edge sites in the catalysis of CO oxidation by a combination of reaction kinetics analysis and DFT calculations. Cu2O nanocrystals undergo insitu surface oxidation forming CuO thin films during CO oxidation. As the average size of the cubic Cu2O nanocrystals decreases from 1029nm to 34nm, the dominant active sites contributing to the catalytic activity switch from face sites to edge sites. These results reveal the interplay between the intrinsic catalytic activity and the density of individual types of surface sites on a catalyst nanoparticle in determining their contributions to the catalytic activity.
引用
收藏
页码:4276 / 4280
页数:5
相关论文
共 30 条
  • [11] Structure Sensitivity of Alkynol Hydrogenation on Shape- and Size-Controlled Palladium Nanocrystals: Which Sites Are Most Active and Selective?
    Crespo-Quesada, Micaela
    Yarulin, Artur
    Jin, Mingshang
    Xia, Younan
    Kiwi-Minsker, Lioubov
    [J]. JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2011, 133 (32) : 12787 - 12794
  • [12] Fluorescence micro(spectro)scopy as a tool to study catalytic materials in action
    De Cremer, Gert
    Sels, Bert F.
    De Vos, Dirk E.
    Hofkens, Johan
    Roeffaers, Maarten B. J.
    [J]. CHEMICAL SOCIETY REVIEWS, 2010, 39 (12) : 4703 - 4717
  • [13] Galwey A.K., 1977, ADV CATAL, V26, P247
  • [14] Atomic-resolution in situ transmission electron microscopy of a promoter of a heterogeneous catalyst
    Hansen, TW
    Wagner, JB
    Hansen, PL
    Dahl, S
    Topsoe, H
    Jacobsen, CJH
    [J]. SCIENCE, 2001, 294 (5546) : 1508 - 1510
  • [15] Hua Q., 2014, Angew. Chem, V126, DOI [10.1002/ange.201402374, DOI 10.1002/ANGE.201402374]
  • [16] Crystal-Plane-Controlled Selectivity of Cu2O Catalysts in Propylene Oxidation with Molecular Oxygen
    Hua, Qing
    Cao, Tian
    Gu, Xiang-Kui
    Lu, Jiqing
    Jiang, Zhiquan
    Pan, Xiaorong
    Luo, Liangfeng
    Li, Wei-Xue
    Huang, Weixin
    [J]. ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2014, 53 (19) : 4856 - 4861
  • [17] Oxide Nanocrystal Model Catalysts
    Huang, Weixin
    [J]. ACCOUNTS OF CHEMICAL RESEARCH, 2016, 49 (03) : 520 - 527
  • [18] Lee I, 2009, NAT MATER, V8, P132, DOI [10.1038/NMAT2371, 10.1038/nmat2371]
  • [19] Facile Synthesis and Shape Evolution of Single-Crystal Cuprous Oxide
    Liang, Xudong
    Gao, Lian
    Yang, Songwang
    Sun, Jing
    [J]. ADVANCED MATERIALS, 2009, 21 (20) : 2068 - 2071
  • [20] Spatially resolved observation of crystal-face-dependent catalysis by single turnover counting
    Roeffaers, MBJ
    Sels, BF
    Uji-i, H
    De Schryver, FC
    Jacobs, PA
    De Vos, DE
    Hofkens, J
    [J]. NATURE, 2006, 439 (7076) : 572 - 575