Title | Direct Identification of Active Surface Species for the Water-Gas Shift Reaction on a Gold-Ceria Catalyst |
Authors | Fu, Xin-Pu Gno, Li-Wen Wang, Wei-Wei Ma, Chao Jia, Chun-Jiang Wu, Ke Si, Rui Sun, Ling-Dong Yan, Chun-Hua |
Affiliation | Shandong Univ, Sch Chem & Chem Engn, Key Lab Special Aggregated Mat, Key Lab Colloid & Interface Chem, Jinan 250100, Shandong, Peoples R China Chinese Acad Sci, Shanghai Inst Appl Phys, Shanghai Synchrotron Radiat Facil, Shanghai 201204, Peoples R China Hunan Univ, Coll Mat Sci & Engn, Changsha 410082, Hunan, Peoples R China Peking Univ, PKU HKU Joint Lab Rare Earth Mat & Bioinorgan Che, State Key Lab Rare Earth Mat Chem & Applicat, Beijing Natl Lab Mol Sci, Beijing 100871, Peoples R China |
Issue Date | 2019 |
Publisher | JOURNAL OF THE AMERICAN CHEMICAL SOCIETY |
Abstract | The crucial role of the metal-oxide interface in the catalysts of the water-gas shift (WGS) reaction has been recognized, while the precise illustration of the intrinsic reaction at the interfacial site has scarcely been presented. Here, two kinds of gold-ceria catalysts with totally distinct gold species, <2 nm clusters and 3 to 4 nm particles, were synthesized as catalysts for the WGS reaction. We found that the gold cluster catalyst exhibited a superiority in reactivity compared to gold nanoparticles. With the aid of comprehensive in situ characterization techniques, the bridged -OH groups that formed on the surface oxygen vacancies of the ceria support are directly determined to be the sole active configuration among various surface hydroxyls in the gold-ceria catalysts. The isotopic tracing results further proved that the reaction between bridged surface -OH groups and CO molecules adsorbed on interfacial Au atoms contributes dominantly to the WGS reactivity. Thus, the abundant interfacial sites in gold clusters on the ceria surface induced superior reactivity compared to that of supported gold nanoparticles in catalyzing the WGS reaction. On the basis of direct and solid experimental evidence, we have obtained a very clear image of the surface reaction for the WGS reaction catalyzed by the gold-ceria catalyst. |
URI | http://hdl.handle.net/20.500.11897/549838 |
ISSN | 0002-7863 |
DOI | 10.1021/jacs.8b09306 |
Indexed | SCI(E) EI |
Appears in Collections: | å å¦ä¸ å å å·¥ç¨ å¦é ¢ 稀土材料化学与应用国家重点实验室 |