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Scale‐Up Biomass Pathway to Cobalt Single‐Site Catalysts Anchored on N‐Doped Porous Carbon Nanobelt with Ultrahigh Surface Area
Authors:Youqi Zhu  Wenming Sun  Wenxing Chen  Tai Cao  Yu Xiong  Jun Luo  Juncai Dong  Lirong Zheng  Jian Zhang  Xiaolu Wang  Chen Chen  Qing Peng  Dingsheng Wang  Yadong Li
Affiliation:1. Department of Chemistry, Tsinghua University, Beijing, China;2. State Key Laboratory of Green Building Materials, China Building Materials Academy, Beijing, China;3. Center for Electron Microscopy, Tianjin University of Technology, Tianjin, China;4. Beijing Synchrotron Radiation Facility, Institute of High Energy Physics, Chinese Academy of Sciences, Beijing, China
Abstract:Porous Co? N? C catalysts with ultrahigh surface area are highly required for catalytic reactions. Here, a scale‐up method to synthesize gram‐quantities of isolated Co single‐site catalysts anchored on N‐doped porous carbon nanobelt (Co‐ISA/CNB) by pyrolysis of biomass‐derived chitosan is reported. The usage of ZnCl2 and CoCl2 salts as effective activation–graphitization agents can introduce a porous belt‐like nanostructure with ultrahigh specific surface area (2513 m2 g?1) and high graphitization degree. Spherical aberration correction electron microscopy and X‐ray absorption fine structure analysis reveal that Co species are present as isolated single sites and stabilized by nitrogen in CoN4 structure. All these characters make Co‐ISA/CNB an efficient catalyst for selective oxidation of aromatic alkanes at room temperature. For oxidation of ethylbenzene, the Co‐ISA/CNB catalysts yield a conversion up to 98% with 99% selectivity, while Co nanoparticles are inert. Density functional theory calculations reveal that the generated Co?O centers on isolated Co single sites are responsible for the excellent catalytic efficiency.
Keywords:2D nanobelt  biomass  cobalt  porous carbon  single‐site catalysts
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