Selective conversion of furfural to cyclopentanone over the N-doped CuNi alloy carbon materials derived from porphyrin-based bimetallic metal-organic frameworks

Zhiquan Cai, Zhiyan Zhang,Yuxuan Qi,Chenglong Zheng, Xuesong Wei,Zhifei Cheng,Yi-Si Feng

Fuel(2024)

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摘要
The creation of CuNi alloys and Pyrrolic-N-Ni bonding facilitated efficient hydrogenation and acid-catalyzed steps of biomass derivatives in aqueous solvents. The carbon materials containing alloys derived from the pyrolysis of bimetallic metal–organic frameworks (MOFs) exhibit a greater dispersion of metal active sites compared to previously prepared reduced metal materials through stirred impregnation. This characteristic guarantees superior hydroreduction activity. Hydrogen (H2) serves a dual role in the tandem reactions, acting both as the reductant during hydrogenation and as a promoter in the acid catalysis step. Our group revealed that the formation of robust chemical bonds (−N-Ni-) between metal-containing species and N-doped carbon supports can promote the utilization of H2 hybridization to generate OHδ--Ni-N-Hδ+ in aqueous. This process modulates the quantity and distribution of acidic sites, leading to a notable enhancement in the rate of acid-catalyzed rearrangement reactions. Hence, the Ni-Cu-NPC catalyst synthesized utilizing bimetallic porphyrin-MOFs fulfills the specified criteria and demonstrates excellent activity, selectivity, and stability in the production of cyclopentanone (CPO) from furfural (FFA).
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关键词
CuNi Alloy,Nitrogen heteroatom,Bimetallic porphyrin-MOFs Furfural,Cyclopentanone
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