Switching Co/N/C Catalysts for Heterogeneous Catalysis and Electrocatalysis by Controllable Pyrolysis of Cobalt Porphyrin
Zhen-Yu Wu,
Ming-Xi Chen,
Sheng-Qi Chu,
Yue Lin,
Hai-Wei Liang,
Jing Zhang,
Shu-Hong Yu
Affiliations
Zhen-Yu Wu
Division of Nanomaterials & Chemistry, Hefei National Laboratory for Physical Sciences at the Microscale, CAS Center for Excellence in Nanoscience, Hefei Science Center of CAS, Collaborative Innovation Center of Suzhou Nano Science and Technology, Department of Chemistry, University of Science and Technology of China, Hefei 230026, China
Ming-Xi Chen
Division of Nanomaterials & Chemistry, Hefei National Laboratory for Physical Sciences at the Microscale, CAS Center for Excellence in Nanoscience, Hefei Science Center of CAS, Collaborative Innovation Center of Suzhou Nano Science and Technology, Department of Chemistry, University of Science and Technology of China, Hefei 230026, China
Sheng-Qi Chu
Institute of High Energy Physics, Chinese Academy of Sciences, Beijing 100049, China
Yue Lin
Division of Nanomaterials & Chemistry, Hefei National Laboratory for Physical Sciences at the Microscale, CAS Center for Excellence in Nanoscience, Hefei Science Center of CAS, Collaborative Innovation Center of Suzhou Nano Science and Technology, Department of Chemistry, University of Science and Technology of China, Hefei 230026, China
Hai-Wei Liang
Division of Nanomaterials & Chemistry, Hefei National Laboratory for Physical Sciences at the Microscale, CAS Center for Excellence in Nanoscience, Hefei Science Center of CAS, Collaborative Innovation Center of Suzhou Nano Science and Technology, Department of Chemistry, University of Science and Technology of China, Hefei 230026, China; Corresponding author
Jing Zhang
Institute of High Energy Physics, Chinese Academy of Sciences, Beijing 100049, China
Shu-Hong Yu
Division of Nanomaterials & Chemistry, Hefei National Laboratory for Physical Sciences at the Microscale, CAS Center for Excellence in Nanoscience, Hefei Science Center of CAS, Collaborative Innovation Center of Suzhou Nano Science and Technology, Department of Chemistry, University of Science and Technology of China, Hefei 230026, China; Corresponding author
Summary: Identifying the optimal synthetic and structural parameters in preparing pyrolyzed metal/nitrogen/carbon (M/N/C) materials is crucial for developing effective catalysts for many important catalytic processes. Here we report a group of mesoporous Co/N/C catalysts ranging from polymerized cobalt porphyrin to Co/N-doped carbons, which are prepared by pyrolysis of cobalt porphyrin using silica nanoparticles as templates at different temperatures, for boosting both heterogeneous catalysis and electrocatalysis. It is revealed that the polymerized cobalt porphyrin prepared at low temperature (500°C) is a polymer-like network with exclusive single-atom Co-Nx sites, and that the high-temperature-pyrolysis (>600°C) produces an electrically conductive Co/N-doped carbon, accompanied by part degradation of Co-Nx centers. We identify that the polymerized cobalt porphyrin with undecomposed Co-Nx centers is optimal for heterogeneous catalytic oxidation of ethylbenzene, whereas the electrically conductive Co/N-doped carbon is ideal for eletrocatalytic oxygen reduction. Our results provide new insights for rationally optimizing M/N/C catalysts for different reactions. : Chemistry; Inorganic Chemistry; Catalysis Subject Areas: Chemistry, Inorganic Chemistry, Catalysis
