期刊
ACS SUSTAINABLE CHEMISTRY & ENGINEERING
卷 10, 期 9, 页码 2947-2959出版社
AMER CHEMICAL SOC
DOI: 10.1021/acssuschemeng.1c07836
关键词
Halogenated nitroarenes; Halogenated aniline; Ni-Sn; Ni-La2O3; d-Band center
资金
- NSFC [22078277, 21908185]
- Project of Hunan Provincial Natural Science Foundation of China [2021JJ30658, 2020JJ5532]
- Degree & Postgraduate Education Reform Project of Hunan Provincial [XDCX2019B095, CX20190489]
- Environment-friendly Chemical Process Integration Technology Hunan Province Key Laboratory
- Collaborative Innovation Center of New Chemical Technologies for Environmental Benignity and Efficient Resource Utilization
In this study, modified MCM-41 supported nickel-based catalysts were used for the hydrogenation of halogenated nitrobenzene. The catalysts modified with Sn or La showed improved catalytic performance, and the mechanism behind it was explained.
Catalytic hydrogenation of nitrocompound is an environment-benign strategy for the production of important aniline intermediates. Herein, MCM-41 was synthesized from sepiolite via an in situ self-assembled method, and the modified MCM-41 supported nickel-based catalysts were prepared and applied in halogenated nitrobenzene hydrogenation to halogenated aniline. As compared to Ni/MCM-41, the Sn- or La-modified MCM-41 supported nickel-based catalysts exhibited better catalytic performance. The electron transfer from Sn or La species to Ni led to a downshift in the d-band center of Ni, which was in favor of H desorption and hence promoted hydrogenation activity. It was found that chloronitrobenzene preferred the tilted adsorption orientation mode on the surface of Ni-Sn and Ni-La2O3 to flat adsorption orientation. Moreover, the C-Cl bond scission on Ni-Sn and Ni-La2O3 was thermodynamically unfavorable in comparison with pure-phased Ni, leading to higher selectivity to chloroaniline. Ni/LaMCM-41-NH2 gave the best catalytic performance of 100% conversion and 99.6% selectivity to m-chloroaniline.
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