|
|||||
|
|
Ordered Porous Nitrogen‐Doped Carbon Matrix with Atomically Dispersed Cobalt Sites as an Efficient Catalyst for Dehydrogenation and Transfer Hydrogenation of N‐Heterocycles |
|
| Authors: | Dr Yunhu Han Dr Ziyun Wang Ruirui Xu Dr Wei Zhang Dr Wenxing Chen Dr Lirong Zheng Jian Zhang Dr Jun Luo Konglin Wu Dr Youqi Zhu Dr Chen Chen Dr Qing Peng Dr Qiang Liu Prof?Dr P Hu Prof?Dr Dingsheng Wang Prof?Dr Yadong Li |
| Institution: | 1. Department of Chemistry, Tsinghua University, Beijing, China;2. School of Chemistry and Chemical Engineering, The Queen's University of Belfast, Belfast, UK;3. School of Chemistry & Chemical Engineering, Shaanxi Normal University, Xi'an, China;4. Beijing Synchrotron Radiation Facility, Institute of High Energy Physics, Chinese Academy of Sciences, Beijing, China;5. Center for Electron Microscopy, Tianjin University of Technology, Tianjin, China |
| Abstract: | Single‐atom catalysts (SACs) have been explored widely as potential substitutes for homogeneous catalysts. Isolated cobalt single‐atom sites were stabilized on an ordered porous nitrogen‐doped carbon matrix (ISAS‐Co/OPNC). ISAS‐Co/OPNC is a highly efficient catalyst for acceptorless dehydrogenation of N‐heterocycles to release H2. ISAS‐Co/OPNC also exhibits excellent catalytic activity for the reverse transfer hydrogenation (or hydrogenation) of N‐heterocycles to store H2, using formic acid or external hydrogen as a hydrogen source. The catalytic performance of ISAS‐Co/OPNC in both reactions surpasses previously reported homogeneous and heterogeneous precious‐metal catalysts. The reaction mechanisms are systematically investigated using first‐principles calculations and it is suggested that the Eley–Rideal mechanism is dominant. |
| Keywords: | atomically dispersed sites dehydrogenation hydrogenation N-doped carbon transfer hydrogenation |