Title | Structural Determination of Catalytically Active Subnanometer Iron Oxide Clusters |
Authors | Yang, Qi Fu, Xin-Pu Jia, Chun-Jiang Ma, Chao Wang, Xu Zeng, Jie Si, Rui Zhang, Ya-Wen Yan, Chun-Hua |
Affiliation | Chinese Acad Sci, Shanghai Inst Appl Phys, Shanghai Synchrotron Radiat Facil, Shanghai 201204, Peoples R China. Shandong Univ, Sch Chem & Chem Engn, Key Lab Special Aggregated Mat, Key Lab Colloid & Interface Chem, Jinan 250100, Peoples R China. Univ Sci & Technol China, Hefei Natl Lab Phys Sci Microscale, Hefei 230026, Anhui, Peoples R China. Peking Univ, PKU HKU Joint Lab Rare Earth Mat & Bioinorgan Che, Beijing Natl Lab Mol Sci, State Key Lab Rare Earth Mat Chem & Applicat, Beijing 100871, Peoples R China. Chinese Acad Sci, Shanghai Inst Appl Phys, Shanghai Synchrotron Radiat Facil, Shanghai 201204, Peoples R China. Jia, CJ (reprint author), Shandong Univ, Sch Chem & Chem Engn, Key Lab Special Aggregated Mat, Key Lab Colloid & Interface Chem, Jinan 250100, Peoples R China. Ma, C (reprint author), Univ Sci & Technol China, Hefei Natl Lab Phys Sci Microscale, Hefei 230026, Anhui, Peoples R China. |
Keywords | subnanometer cluster iron-ceria active site metal-support interaction structure-activity relationship FISCHER-TROPSCH SYNTHESIS GAS SHIFT REACTION CO OXIDATION MIXED OXIDES IN-SITU CATALYSTS GOLD SIZE NANOPARTICLES CARBIDE |
Issue Date | 2016 |
Publisher | ACS CATALYSIS |
Citation | ACS CATALYSIS.2016,6,(5),3072-3082. |
Abstract | Supported subnanometer clusters exhibit superiority in catalytic performance compared to common nanoparticles, due to their higher fraction of exposed surfaces and larger number of active species at the metal support interface, responding to the size effect and the support effect in heterogeneous catalysis. Here, we report the synthesis of subnanometer iron oxide clusters anchored to the surfaces of two types of ceria nanoshapes (nanorods and nanopolyhedra), as well as the structure activity relation investigation for Fischer-Tropsch synthesis. On the basis of the comprehensive structural characterizations including aberration-corrected scanning transmission electron microscopy (STEM) and X-ray absorption fine structure (XAFS), we demonstrated that the subnanometer clusters of iron oxide are stable and catalytically active for the Fischer-Tropsch synthesis reaction. Furthermore, it is identified that finely dispersed iron oxide clusters (Fe-O-x-Fe-y) consisted of partially reduced Fe delta+ (delta = 2.6-2.9) species in ceria nanorods are active for Fischer Tropsch synthesis; however, another type of iron oxide cluster (Fe-O-x-Ce-y) composed of fully oxidized Fe3+ ions strongly interacted with the ceria nanopolyhedra support but exhibits relatively poorer activity for the reaction. These results have broad implications on the fundamental understanding of active site of supported metal catalysts at the atomic level. |
URI | http://hdl.handle.net/20.500.11897/437276 |
ISSN | 2155-5435 |
DOI | 10.1021/acscatal.6b00328 |
Indexed | SCI(E) EI |
Appears in Collections: | 化学与分子工程学院 稀土材料化学与应用国家重点实验室 |