MOF-derived N-doped carbon composites embedded with Fe/Fe3C nanoparticles as highly chemoselective and stable catalysts for catalytic transfer hydrogenation of nitroarenes

被引:46
作者
Feng, Binbin [1 ]
Xu, Qionghao [1 ]
Wu, Xiaoxue [1 ]
Ye, Chunlin [1 ]
Fu, Yanghe [1 ]
Chen, De-Li [1 ]
Zhang, Fumin [1 ]
Zhu, Weidong [1 ]
机构
[1] Zhejiang Normal Univ, Inst Phys Chem, Key Lab, Minist Educ Adv Catalysis Mat, Jinhua 321004, Zhejiang, Peoples R China
基金
中国国家自然科学基金;
关键词
Metal-organic framework; Fe; Fe3C@NC; Nitrogen-doped porous carbon; Selective catalytic hydrogenation; Nitro compounds; METAL-ORGANIC FRAMEWORKS; POROUS CARBON; ROOM-TEMPERATURE; REDUCTION; PERFORMANCE; EFFICIENT; NITROBENZENE; ELECTROCATALYSTS; NH2-MIL-101(FE); NANOCOMPOSITES;
D O I
10.1016/j.apsusc.2021.149837
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Owing to the competitive hydrogenation of reducible functionalized groups and the complexity of the reaction mechanism, the selective catalytic hydrogenation of nitroarene compounds to value-added amine products is challenging. Herein, we designed and prepared a series of highly efficient iron-based nanocomposites (Fe/ Fe3C@NC-T) via direct pyrolysis of the presynthesized NH2-MIL-101(Fe) octahedrons under nitrogen atmosphere, wherein tiny metallic Fe/Fe3C nanoparticles (NPs) were homogeneously inlaid in the N-doped porous carbon matrix. Among the various derived catalysts, Fe/Fe3C@NC-750 exhibited the best performance, with good tolerance to several different functional groups for the catalytic transfer hydrogenation of nitroarenes to anilines using N2H4 center dot H2O as the reductant under mild conditions. This performance was also superior to those of commercial catalysts (Fe, Fe2O3, and Fe3C) and Fe/Fe3C@C-750 without N doping. The synergistic catalysis between the Fe-based NP and N dopant mainly contributed to the excellent catalytic performance of Fe/ Fe3C@NC-750. Moreover, the mechanism study revealed that both the direct route and the condensation route were involved in this catalytic reaction system.
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页数:11
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