Journal
MOLECULAR CATALYSIS
Volume 477, Issue -, Pages -Publisher
ELSEVIER
DOI: 10.1016/j.mcat.2019.110544
Keywords
Metal-organic frameworks; N-Doped carbon fiber; FeOx-based catalysts; Electrospun; Hydrogenation of nitroarenes
Categories
Funding
- National Natural Science Foundation of China [21471051]
- Doctoral Fund of Ministry of Education of China [2017M621315]
- Heilongjiang Provincial Government Postdoctoral Science Foundation [LBH-Z17190]
- State Key Laboratory of Fine Chemicals [KF1714]
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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 FeOx-based nanocatalyst (FeOx@CN-hpes) was prepared via pyrolysis of MOF@polymer composite towards electrospun nanofiber crosslinked N, Fe-containing MOFs. Remarkably, the developed FeOx@CN-hpes enables the hydrogenation of nitrobenzene to aniline with unprecedented performance (215.8 h(-1)) compared to those of FeOx@CN-hp (176.2 h(-1)) and FeOx@CN-pes (45.2 h(-1)) catalysts prepared by conventional approaches. The comparative characterizations have revealed that the high dispersion of FeOx species, enhanced basicity, and more structural defects and Fe-N-x species towards FeOx@CN-hpes are responsible for the high performance. Moreover, the effect of the pyrolysis temperature towards FeOx@CN-hpes on the performance of hydrogenation reaction was also systematically investigated. The results indicated that the FeOx@CN-hpes-400 catalyst prepared at 400 degrees C was identified as the best hydrogenation catalyst. More importantly, the FeOx@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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