MIL-53 (Al) derived single-atom Rh catalyst for the selective hydrogenation of m-chloronitrobenzene into m-chloroaniline

نویسندگان

چکیده

The catalytic hydrogenation of halonitroarenes to haloanilines is a green and sustainable process for the production key nitrogen-containing intermediates in fine chemical industry. Chemoselective poses significant challenge, which requires rational design catalysts with proper ability nitro group simultaneously preventing dehalogenation halogen group. Herein, highly effective Rh@Al 2 O 3 @C single-atom catalyst (SAC) was developed m -chloronitrobenzene ( -CNB) -chloroaniline -CAN), through an in-situ grafting metal during assembly MIL-53 (Al), followed by confined pyrolysis. Extensive characterizations reveal exquisite structure @C, containing atomically dispersed Rh sites onto Al amorphous carbon. five-coordinated aluminum (Al V ) species are essential achieving atomic dispersion atoms, providing unsaturated coordinative metal. Compared benchmark Rh/γ-Al Rh/C nanocatalysts, SAC affords excellent turnover frequency 2317 mol -CNB ·mol –1 ·h , highest value date heterogeneous systems at 313 K 20 bar H together sustained selectivity -CAN (~98%) five consecutive runs. superior performance attributed modulation electronic forming SAC, enhanced accessibility acid function sites. Rh@Al2O3@C fabricated utilizing metal-organic framework shows excellent, chemoselectivity m-chloronitrobenzene.

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ژورنال

عنوان ژورنال: Chinese Journal of Catalysis

سال: 2021

ISSN: ['0253-9837', '1872-2067']

DOI: https://doi.org/10.1016/s1872-2067(20)63697-x