期刊
ADVANCED FUNCTIONAL MATERIALS
卷 28, 期 37, 页码 -出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/adfm.201802167
关键词
2D nanobelt; biomass; cobalt; porous carbon; single-site catalysts
类别
资金
- China Ministry of Science and Technology [2016YFA (0202801)]
- National Natural Science Foundation of China [21521091, 21390393, U1463202, 21471089, 21671117, 21703219]
- China Postdoctoral Science Foundation [2017M620738]
Porous CoNC 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 m(2) 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.
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