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Co embedded within biomass-derived mesoporous N-doped carbon as an acid-resistant and chemoselective catalyst for transfer hydrodeoxygenation of biomass with formic acid

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Abstract

An N-doped Co@C catalyst (Co@NC) is synthesized by a one-pot carbonization of biomass-derived glucose and harmless melamine with CoCl2 as the catalyst, where C and N resources could be transformed into highly graphitic N-doped carbon, while the coordinated Co2+ ions are reduced to uniform Co nanoparticles (NPs), which are embedded in N-doped graphitic structures. Under base-free conditions with formic acid (FA) as a hydrogen donor, the optimized Co@NC-700 (pyrolyzed at 700 °C) shows a highly efficient H2 generation from FA and the best activity for vanillin hydrodeoxygenation (HDO) with FA. For example, Co@NC-700 exhibits 15.4 times higher activity in comparison with uncovered Co on AC (Co/AC), and affords >95% vanillin conversion with 2-methoxy-4-methylphenol (MMP) as the sole product at 180 °C for 4 h. Compared with molecular hydrogen, Co@NC-700 gives a much higher activity and MMP selectivity for vanillin HDO with FA. The Co@NC-700 demonstrates enhanced acid resistance in acidic medium and adsorption of vanillin, and is recyclable and versatile for hydrogenating various unsaturated compounds. The superior performance of Co@NC-700 could be ascribed to N-derived defective sites on Co@NC, which could play multiple roles as base additives in FA dehydrogenation and as a metal-like active center in vanillin HDO.

Graphical abstract: Co embedded within biomass-derived mesoporous N-doped carbon as an acid-resistant and chemoselective catalyst for transfer hydrodeoxygenation of biomass with formic acid

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Publication details

The article was received on 30 Aug 2017, accepted on 26 Oct 2017 and first published on 26 Oct 2017


Article type: Paper
DOI: 10.1039/C7GC02648J
Citation: Green Chem., 2017, Advance Article
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    Co embedded within biomass-derived mesoporous N-doped carbon as an acid-resistant and chemoselective catalyst for transfer hydrodeoxygenation of biomass with formic acid

    H. Yang, R. Nie, W. Xia, X. Yu, D. Jin, X. Lu, D. Zhou and Q. Xia, Green Chem., 2017, Advance Article , DOI: 10.1039/C7GC02648J

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