Biomass-derived 2D Pb^(0)/Pb^(2+) dual-center-site catalysts for efficient 5 hydroxymethylfurfural electroreduction  

作　　者：Haoran Wu Haishan Xu Zhenbing Xie Runlu Yang Xin Wang Xinwei Chen Liang Wu Chongyin Zhang Weixia Zhu Yiyong Mai 

机构地区：[1]School of Chemical Engineering,Zhengzhou University,Zhengzhou 450001,China [2]School of Chemistry and Chemical Engineering,Frontiers Science Center for Transformative Molecules,Shanghai Key Laboratory of Electrical Insulation and Thermal Ageing,Shanghai Jiao Tong University,Shanghai 200240,China [3]Department of Chemistry,Tangshan Normal University,Tangshan 063000,China [4]Shanghai Aerospace Equipments Manufacturer Co.,Ltd.,Shanghai 200245,China

出　　处：《Nano Research》2025年第2期101-110,共10页纳米研究(英文版)

基　　金：This work was supported by the National Natural Science Foundation of China(Nos.22225501 and 52073173);the Key Research Projects of Universities in Henan Province(No.23A530005);the National Key Laboratory of Biobased Transport Fuel Technology(No.KFKT2022002)of China;Program of Shanghai Academic/Technology Research Leader(No.23XD1431700);Shanghai Engineering Research Center of Specialized Polymer Materials for Aerospace(No.18DZ2253500).

摘　　要：Using natural resources to construct electrocatalysts for biomass conversion and elucidating their catalytic mechanisms are of great significance,but have remained challenging.Here,a series of two-dimensional(2D)biomass-based Pb/PbO@C nanoparticles catalysts with Pb/PbO anchored on carbon nanosheets were synthesized using natural-derived humate as the precursor.By adjusting the carbonization temperature,an electron-deficient Pb0/Pb^(2+)dual-center-site catalyst can be achieved.The optimized Pb/PbO@C catalyst showed an excellent performance for the electrochemical hydrogenation of 5 hydroxymethylfurfural(HMF)to high value-added 2,5 bis(hydroxymethyl)furan(BHMF),with high Faradaic efficiency(FE:91.9%)and selectivity(Sel:89.7%),achieving comparable performance to those of the reported noble metal-based electrocatalysts.Mechanism study revealed that the electron-deficient Pb^(0)/Pb^(2+)dual-center-site provided abundant Lewis acidic sites and promoted the dissociation of water to the active hydrogen(H^(*))species,thus enhancing the adsorption of HMF on Pb^(2+)sites and the coverage of H^(*)species on Pb0 sites.The high coverage of H*species and the synergistic effect of dual-center sites substantially promoted the binding of H*and HMF to form H-HMF^(*)and inhibited the recombination of H^(*)species,thereby accelerating the reaction kinetics of HMF reduction.

关 键 词：biomass conversion biomass-derived carbon materials electrocatalysis hydrogenation 5 hydroxymethylfurfural 

分 类 号：O64[理学—物理化学]