Metal-free carbocatalyst for catalytic hydrogenation of N-containing unsaturated compounds
| Autor: | Zhaolin He, Chuyi Xie, Junxia Yu, Chunyan Tang, Qijun Wang, Jun Chen, Zhipan Wen, Meng Zhao, Devaraj Manoj, Jin Liu, Jiangbo Xi, Zhengwu Bai, Shuai Wang |
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| Rok vydání: | 2019 |
| Předmět: |
010405 organic chemistry
Chemistry Graphene Oxide Chromophore 010402 general chemistry 01 natural sciences Redox Catalysis Hydrothermal circulation 0104 chemical sciences law.invention chemistry.chemical_compound Chemical engineering law Specific surface area Molecule Physical and Theoretical Chemistry |
| Zdroj: | Journal of Catalysis. 377:199-208 |
| ISSN: | 0021-9517 |
| DOI: | 10.1016/j.jcat.2019.07.017 |
| Popis: | 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 m2 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 × 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. |
| Databáze: | OpenAIRE |
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