Unraveling Charge State of Supported Au Single-Atoms during CO Oxidation

被引：227

作者：

Zhou, Xiong ^{[1
,2
]}

Shen, Qian ^{[1
,2
]}

Yuan, Kaidi ^{[2
]}

Yang, Wenshao ^{[3
]}

Chen, Qiwei ^{[1
]}

Geng, Zhenhua ^{[3
]}

Zhang, Jialin ^{[2
]}

Shao, Xiang ^{[4
]}

Chen, Wei ^{[2
]}

Xu, Guoqin ^{[2
]}

Yang, Xueming ^{[3
]}

Wu, Kai ^{[1
]}

机构：

[1] Peking Univ, Coll Chem & Mol Engn, BNLMS, Beijing 100871, Peoples R China

[2] Natl Univ Singapore, Dept Chem, Singapore 117543, Singapore

[3] Dalian Inst Chem Phys, State Key Lab Mol React Dynam, Dalian 116023, Liaoning, Peoples R China

[4] Univ Sci & Technol China, Sch Chem & Mat Sci, Dept Chem Phys, Hefei 230026, Anhui, Peoples R China

来源：

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY | 2018年 / 140卷 / 02期

关键词：

CATALYTIC SITES; GOLD CLUSTERS; ACTIVE-SITES; AU/TIO2; SURFACE; RECONSTRUCTION; NANOCLUSTERS; MECHANISM; CATIONS; CERIA;

D O I：

10.1021/jacs.7b10394

中图分类号：

O6 [化学];

学科分类号：

0703 ;

摘要：

Thermally stable Au single-atoms supported by monolayered CuO grown at Cu(110) have been successfully prepared. The charge transfer from the CuO support to single Au atoms is confirmed to play a key role in, tuning the activity for CO oxidation. Initially, the negatively charged Au single-atom is active for CO oxidation with its adjacent lattice O atom depleted to generate an O vacancy in the CuO monolayer. Afterward, the Au single-atom is neutralized, preventing further CO reaction. The produced O vacancy can be healed by exposure to O-2 at 400 K and accordingly the reaction activity is restored.

引用

页码：554 / 557

页数：4

共 47 条

[1] Chemical tip fingerprinting in scanning probe microscopy of an oxidized Cu(110) surface [J].

Bamidele, J. ;

Kinoshita, Y. ;

Turansky, R. ;

Lee, S. H. ;

Naitoh, Y. ;

Li, Y. J. ;

Sugawara, Y. ;

Stich, I. ;

Kantorovich, L. .

PHYSICAL REVIEW B, 2012, 86 (15)

[2] Oxidation-resistant gold-55 clusters [J].

Boyen, HG ;

Kästle, G ;

Weigl, F ;

Koslowski, B ;

Dietrich, C ;

Ziemann, P ;

Spatz, JP ;

Riethmüller, S ;

Hartmann, C ;

Möller, M ;

Schmid, G ;

Garnier, MG ;

Oelhafen, P .

SCIENCE, 2002, 297 (5586) :1533-1536

[3] Reaction Mechanisms for the CO Oxidation on Au/CeO2 Catalysts: Activity of Substitutional Au3+/Au+ Cations and Deactivation of Supported Au+ Adatoms [J].

Camellone, Matteo Farnesi ;

Fabris, Stefano .

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2009, 131 (30) :10473-10483

[4] Catalytically active gold: From nanoparticles to ultrathin films [J].

Chen, Mingshu ;

Goodman, D. Wayne .

ACCOUNTS OF CHEMICAL RESEARCH, 2006, 39 (10) :739-746

[5] NOVEL MECHANISM FOR THE FORMATION OF CHEMISORPTION PHASES - THE (2X1)O-CU(110 ADDED-ROW RECONSTRUCTION [J].

COULMAN, DJ ;

WINTTERLIN, J ;

BEHM, RJ ;

ERTL, G .

PHYSICAL REVIEW LETTERS, 1990, 64 (15) :1761-1764

[6] Effect of postgrowth oxygen exposure on the magnetic properties of Ni on the Cu-CuO stripe phase [J].

Denk, M. ;

Denk, R. ;

Hohage, M. ;

Sun, L. D. ;

Zeppenfeld, P. .

PHYSICAL REVIEW B, 2012, 85 (01)

[7] Gold Atoms Stabilized on Various Supports Catalyze the Water-Gas Shift Reaction [J].

Flytzani-Stephanopoulos, Maria .

ACCOUNTS OF CHEMICAL RESEARCH, 2014, 47 (03) :783-792

[8] Active nonmetallic Au and Pt species on ceria-based water-gas shift catalysts [J].

Fu, Q ;

Saltsburg, H ;

Flytzani-Stephanopoulos, M .

SCIENCE, 2003, 301 (5635) :935-938

[9] Surface Science Investigations of Oxidative Chemistry on Gold [J].

Gong, Jinlong ;

Mullins, C. Buddie .

ACCOUNTS OF CHEMICAL RESEARCH, 2009, 42 (08) :1063-1073

[10] Spectroscopic Observation of Dual Catalytic Sites During Oxidation of CO on a Au/TiO2 Catalyst [J].

Green, Isabel Xiaoye ;

Tang, Wenjie ;

Neurock, Matthew ;

Yates, John T., Jr. .

SCIENCE, 2011, 333 (6043) :736-739

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