Affiliation: | 1. State Key Laboratory of Rare Earth Resource Utilization, Changchun Institute of Applied Chemistry, Chinese Academy of Sciences, Changchun, 130022 China School of Applied Chemistry and Engineering, University of Science and Technology of China, Hefei, 230026 China;2. State Key Laboratory of Rare Earth Resource Utilization, Changchun Institute of Applied Chemistry, Chinese Academy of Sciences, Changchun, 130022 China;3. Center for Nanoparticle Research, Institute for Basic Science (IBS), Seoul, 08826 Republic of Korea School of Chemical and Biological Engineering, and Institute of Chemical Processes, Seoul National University, Seoul, 08826 (Republic of Korea;4. Center for Nanoparticle Research, Institute for Basic Science (IBS), Seoul, 08826 Republic of Korea;5. Shanghai Synchrotron Radiation Facility, Zhangjiang Laboratory, Shanghai Advanced Research Institute, Chinese Academy of Sciences, Shanghai, 201204 China |
Abstract: | Reducible oxide-supported noble metal nanoparticles exhibit high activity in catalyzing many important oxidation reactions. However, atom migration under harsh reaction conditions leads to deactivation of the catalyst. Meanwhile, single-atom catalysts demonstrate enhanced stability, but often suffer from poor catalytic activity owing to the ionized surface states. In this work, we simultaneously address the poor activity and stability issues by synthesizing highly active and durable rhodium (Rh) single-atom catalysts through a “wrap-bake-peel” process. The pre-coated SiO2 layer during synthesis of catalyst plays a crucial role in not only protecting CeO2 support against sintering, but also donating electron to weaken the Ce−O bond, producing highly loaded Rh single atoms on the CeO2 support exposed with high-index {210} facets. Benefiting from the unique electronic structure of CeO2 {210} facets, more oxygen vacancies are generated along with the deposition of more electropositive Rh single atoms, leading to remarkably improved catalytic performance in CO oxidation. |