Journal
JOURNAL OF CATALYSIS
Volume 377, Issue -, Pages 199-208Publisher
ACADEMIC PRESS INC ELSEVIER SCIENCE
DOI: 10.1016/j.jcat.2019.07.017
Keywords
Carbocatalyst; Nitrogen doped holey graphene; Hydrogenation; Organic dye; Density functional theory
Categories
Funding
- Natural Science Foundation of Hubei Province [2016CFB263, 2016CFB168, 2018CFB159]
- National Natural Science Foundation of China [21702155, 51772110, 51708427]
- Analytical and Testing Center of Huazhong University of Science and Technology
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Eco-friendly carbocatalyst is extremely desirable in organic catalysis and wastewater treatment. Herein, we reported a one-pot synchronous hydrothermal process to synthesize a highly efficient N doped holey graphene (NHG) carbocatalyst, in which graphene oxide nanosheets are self-assembled, reduced, chemically etched, and simultaneously doped with nitrogen to form a graphene hydrogel in the presence of H2O2 and NH4OH. Benefiting from the good hydrophilicity, unique hierarchical porous structure, large specific surface area (322.1 m(2)g(-1)), and high N content (9.77 at. %), the resultant NHG carbocatalyst exhibits an excellent catalytic performance for the hydrogenation of N-containing unsaturated compounds. In 4-nitrophenol reduction reaction, the NHG carbocatalyst delivers a turnover frequency of 3.32 x 10(-2) min(-1). This catalytic activity is superior to that of the commercial Pd/C (5.0 wt%), other previously reported carbocatalysts, and many noble-metal-based catalysts. Furthermore, the molecular structure analysis combined with density functional theory calculations elucidate metal-free catalytic mechanism of hydrogenation reaction for unsaturated chromophore groups in N-containing organic dyes. (C) 2019 Elsevier Inc. All rights reserved.
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