In situ manipulation of the active Au-TiO2 interface with atomic precision during CO oxidation

被引:224
作者
Yuan, Wentao [1 ,2 ]
Zhu, Beien [3 ,4 ]
Fang, Ke [1 ,2 ]
Li, Xiao-Yan [4 ,5 ]
Hansen, Thomas W. [6 ]
Ou, Yang [1 ,2 ]
Yang, Hangsheng [1 ,2 ]
Wagner, Jakob B. [6 ]
Gao, Yi [3 ,4 ]
Wang, Yong [1 ,2 ]
Zhang, Ze [1 ,2 ]
机构
[1] Zhejiang Univ, State Key Lab Silicon Mat, Sch Mat Sci & Engn, Hangzhou 310027, Peoples R China
[2] Zhejiang Univ, Ctr Electron Microscopy, Sch Mat Sci & Engn, Hangzhou 310027, Peoples R China
[3] Chinese Acad Sci, Interdisciplinary Res Ctr, Shanghai Adv Res Inst, Zhangjiang Lab, Shanghai 201210, Peoples R China
[4] Chinese Acad Sci, Shanghai Inst Appl Phys, Key Lab Interfacial Phys & Technol, Shanghai 201800, Peoples R China
[5] Univ Chinese Acad Sci, Beijing 100049, Peoples R China
[6] Tech Univ Denmark, DTU Nanolab, DK-2800 Lyngby, Denmark
基金
中国博士后科学基金; 中国国家自然科学基金;
关键词
TOTAL-ENERGY CALCULATIONS; ELECTRON-MICROSCOPY; CATALYTIC-ACTIVITY; GOLD CLUSTERS; NANOPARTICLES; HYDROGEN; PERCENTAGE; TITANIA; SURFACE; OXYGEN;
D O I
10.1126/science.abe3558
中图分类号
O [数理科学和化学]; P [天文学、地球科学]; Q [生物科学]; N [自然科学总论];
学科分类号
07 ; 0710 ; 09 ;
摘要
The interface between metal catalyst and support plays a critical role in heterogeneous catalysis. An epitaxial interface is generally considered to be rigid, and tuning its intrinsic microstructure with atomic precision during catalytic reactions is challenging. Using aberration-corrected environmental transmission electron microscopy, we studied the interface between gold (Au) and a titanium dioxide (TiO2) support. Direct atomic-scale observations showed an unexpected dependence of the atomic structure of the Au-TiO2 interface with the epitaxial rotation of gold nanoparticles on a TiO2 surface during carbon monoxide (CO) oxidation. Taking advantage of the reversible and controllable rotation, we achieved in situ manipulation of the active Au-TiO2 interface by changing gas and temperature. This result suggests that real-time design of the catalytic interface in operating conditions may be possible.
引用
收藏
页码:517 / +
页数:23
相关论文
共 48 条
[1]   Electron Microscopy Study of Gold Nanoparticles Deposited on Transition Metal Oxides [J].
Akita, Tomoki ;
Kohyama, Masanori ;
Haruta, Masatake .
ACCOUNTS OF CHEMICAL RESEARCH, 2013, 46 (08) :1773-1782
[2]   PROJECTOR AUGMENTED-WAVE METHOD [J].
BLOCHL, PE .
PHYSICAL REVIEW B, 1994, 50 (24) :17953-17979
[3]  
Chase MW Jr, 1998, NIST-JANAF thermochemical tables
[4]   Recent advances in understanding CO oxidation on gold nanoparticles using density functional theory [J].
Chen, Ying ;
Crawford, Paul ;
Hu, P. .
CATALYSIS LETTERS, 2007, 119 (1-2) :21-28
[5]   Chemoselective hydrogenation of nitro compounds with supported gold catalysts [J].
Corma, Avelino ;
Serna, Pedro .
SCIENCE, 2006, 313 (5785) :332-334
[6]   Atomic-scale electron microscopy at ambient pressure [J].
Creemer, J. F. ;
Helveg, S. ;
Hoveling, G. H. ;
Ullmann, S. ;
Molenbroek, A. M. ;
Sarro, P. M. ;
Zandbergen, H. W. .
ULTRAMICROSCOPY, 2008, 108 (09) :993-998
[7]   Nanoscale chemical imaging of a working catalyst by scanning transmission X-ray microscopy [J].
de Smit, Emiel ;
Swart, Ingmar ;
Creemer, J. Fredrik ;
Hoveling, Gerard H. ;
Gilles, Mary K. ;
Tyliszczak, Tolek ;
Kooyman, Patricia J. ;
Zandbergen, Henny W. ;
Morin, Cynthia ;
Weckhuysen, Bert M. ;
de Groot, Frank M. F. .
NATURE, 2008, 456 (7219) :222-U39
[8]   Mechanism and Active Sites of the Oxidation of CO over Au/TiO2 [J].
Fujitani, Tadahiro ;
Nakamura, Isao .
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2011, 50 (43) :10144-10147
[9]   Interfaces in Heterogeneous Catalysts: Advancing Mechanistic Understanding through Atomic-Scale Measurements [J].
Gao, Wenpei ;
Hood, Zachary D. ;
Chi, Miaofang .
ACCOUNTS OF CHEMICAL RESEARCH, 2017, 50 (04) :787-795
[10]   Catalytic Activities of Subnanometer Gold Clusters (Au16-Au18, Au20, and Au27-Au35) for CO Oxidation [J].
Gao, Yi ;
Shao, Nan ;
Pei, Yong ;
Chen, Zhongfang ;
Zeng, Xiao Cheng .
ACS NANO, 2011, 5 (10) :7818-7829