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Biomass-derived N-doped porous carbon: an efficient metal-free catalyst for methylation of amines with CO2

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Abstract

Developing green, efficient, and low-cost catalysts for methylation of N–H by using CO2 as the C1 resource is highly desired yet remains a significant challenge. Herein, N-doped porous carbons (NPCs) were designed, synthesized, and proved to be an excellent metal-free catalyst for CO2-participated methylation conversion. NPCs were prepared via the pyrolysis of a mixture of tannic acid and urea. Both theoretical calculation and experiment demonstrate that the N species especially pyridinic N and pyrrolic N within NPCs can work as Lewis basic sites for attacking CO2 to weaken the C[double bond, length as m-dash]O bonds and lower the molecule conversion barrier, facilitating the subsequent methylation of N–H to produce, for example, N,N-dimethylaniline. Besides, the unique porous structure can enrich CO2 and accelerate mass transfer, synergistically promoting the conversion of CO2. The optimized NPC(1/5) catalyst, integrating the porous structure and strong Lewis basicity, exhibits excellent catalytic activity for CO2-based methylation reaction under mild conditions (1 bar CO2, 75 °C). Our work, for the first time, demonstrates the feasibility of using NPCs to catalyze the methylation of amino compounds to produce N,N-dimethylamine by exploiting CO2 as the C1 resource.

Graphical abstract: Biomass-derived N-doped porous carbon: an efficient metal-free catalyst for methylation of amines with CO2

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Publication details

The article was received on 18 Sep 2019, accepted on 30 Oct 2019 and first published on 05 Nov 2019


Article type: Communication
DOI: 10.1039/C9GC03277K
Green Chem., 2019, Advance Article

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    Biomass-derived N-doped porous carbon: an efficient metal-free catalyst for methylation of amines with CO2

    F. Tang, L. Wang and Y. Liu, Green Chem., 2019, Advance Article , DOI: 10.1039/C9GC03277K

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