Enhancing the Electrocatalytic Oxidation of 5-Hydroxymethylfurfural Through Cascade Structure Tuning for Highly Stable Biomass Upgrading  

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作  者:Xiaoli Jiang Xianhui Ma Yuanteng Yang Yang Liu Yanxia Liu Lin Zhao Penglei Wang Yagang Zhang Yue Lin Yen Wei 

机构地区:[1]School of Materials and Energy,University of Electronic Science and Technology of China,Chengdu 611731,People’s Republic of China [2]Hefei National Research Center for Physical Sciences at the Microscale,University of Science and Technology of China,Hefei 230026,People’s Republic of China [3]The Key Laboratory of Bioorganic Phosphorus Chemistry and Chemical Biology(Ministry of Education),Department of Chemistry,Tsinghua University,Beijing 100084,People’s Republic of China [4]School of Materials Science and Engineering,North Minzu University,Yinchuan 750021,People’s Republic of China

出  处:《Nano-Micro Letters》2024年第12期449-467,共19页纳微快报(英文版)

基  金:financially supported by Key Research and Development Projects of Sichuan Province (2023YFG0222);“Tianfu Emei” Science and Technology Innovation Leader Program in Sichuan Province (2021);University of Electronic Science and Technology of China Talent Start-up Funds (A1098 5310 2360 1208);the Youth Innovation Promotion Association of CAS (2020458);National Natural Science Foundation of China (21464015, 21472235, 52122212, 12274391, 223210001);Beijing Natural Science Foundation (IS23045)

摘  要:Electrocatalytic 5-hydroxymethylfurfural oxidation reaction(HMFOR)provides a promising strategy to convert biomass derivative to highvalue-added chemicals.Herein,a cascade strategy is proposed to construct Pd-NiCo_(2)O_(4)electrocatalyst by Pd loading on Ni-doped Co3O4 and for highly active and stable synergistic HMF oxidation.An elevated current density of 800 mA cm^(-2)can be achieved at 1.5 V,and both Faradaic efficiency and yield of 2,5-furandicarboxylic acid remained close to 100%over 10 consecutive electrolysis.Experimental and theoretical results unveil that the introduction of Pd atoms can modulate the local electronic structure of Ni/Co,which not only balances the competitive adsorption of HMF and OH-species,but also promote the active Ni^(3+)species formation,inducing high indirect oxidation activity.We have also discovered that Ni incorporation facilitates the Co2+pre-oxidation and electrophilic OH*generation to contribute direct oxidation process.This work provides a new approach to design advanced electrocatalyst for biomass upgrading.

关 键 词:5-Hydroxymethylfurfural oxidation reaction Competitive adsorption Cascade strategy Elevated current density 

分 类 号:TQ426[化学工程] TQ251.11

 

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