摘要
Rational design and development of stable nitrogen-doped carbon supported non-noble metal based nanocatalysts with unique natures of active species and support for highly chemoselective hydrogenation of nitroarenes to arylamines remains a grand challenge. Here, firstly, an N, Fe-containing metal-organic frameworks (MOFs) has been designed and synthesized. Furthermore, an efficient N-doped carbon fiber supported FeO x -based nanocatalyst (FeO x @CN- hpes ) was prepared via pyrolysis of MOF@polymer composite towards electrospun nanofiber crosslinked N, Fe-containing MOFs. Remarkably, the developed FeO x @CN- hpes enables the hydrogenation of nitrobenzene to aniline with unprecedented performance (215.8 h −1 ) compared to those of FeO x @CN- hp (176.2 h −1 ) and FeO x @CN- pes (45.2 h −1 ) catalysts prepared by conventional approaches. The comparative characterizations have revealed that the high dispersion of FeO x species, enhanced basicity, and more structural defects and Fe-N x species towards FeO x @CN- hpes are responsible for the high performance. Moreover, the effect of the pyrolysis temperature towards FeO x @CN- hpes on the performance of hydrogenation reaction was also systematically investigated. The results indicated that the FeO x @CN- hpes -400 catalyst prepared at 400 °C was identified as the best hydrogenation catalyst. More importantly, the FeO x @CN- hpes -400 catalyst exhibited excellent activity and exclusive selectivity for the hydrogenation of functionalized nitroarenes to corresponding arylamines, as well as successive recyclability without any loss in both activity and selectivity. Therefore, this work provides a feasible strategy for the synthesis of other heterogeneous MOFs-based derived catalysts with superior catalytic performance for diverse industrial processes.
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