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负载型单原子催化剂促进氢氧根吸附用于低浓度碱性电解液中的5-羟甲基糠醛电氧化(英文)

Electro-oxidation of 5-hydroxymethylfurfural in a low-concentrated alkaline electrolyte by enhancing hydroxyl adsorption over a single-atom supported catalyst

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【作者】 夏晓霞徐静怡于欣茹杨静李岸臻纪凯悦李磊马敏邵谦葛瑞翔段昊泓

【Author】 Xiaoxia Xia;Jingyi Xu;Xinru Yu;Jing Yang;An-Zhen Li;Kaiyue Ji;Lei Li;Min Ma;Qian Shao;Ruixiang Ge;Haohong Duan;College of Chemical and Biological Engineering, Shandong University of Science and Technology;Department of Chemistry, Tsinghua University;Hefei National Research Center for Physical Sciences at the Microscale, University of Science and Technology of China;College of Materials Science and Engineering, Shandong University of Science and Technology;

【通讯作者】 葛瑞翔;段昊泓;

【机构】 College of Chemical and Biological Engineering, Shandong University of Science and TechnologyDepartment of Chemistry, Tsinghua UniversityHefei National Research Center for Physical Sciences at the Microscale, University of Science and Technology of ChinaCollege of Materials Science and Engineering, Shandong University of Science and Technology

【摘要】 Electrocatalytic oxidation of 5-hydroxymethylfurfural (HMF) to 2,5-furandicarboxylic acid (FDCA),a sustainable strategy to produce bio-based plastic monomer,is always conducted in a high-concentration alkaline solution (1.0 mol L-1KOH) for high activity.However,such high concentration of alkali poses challenges including HMF degradation and high operation costs associated with product separation.Herein,we report a single-atom-ruthenium supported on Co3O4(Ru1-Co3O4) as a catalyst that works efficiently in a low-concentration alkaline electrolyte (0.1 mol L-1KOH),exhibiting a low potential of 1.191 V versus a reversible hydrogen electrode to achieve 10 m A cm-2 in 0.1 mol L-1 KOH,which outperforms previous catalysts.Electrochemical studies demonstrate that single-atom-Ru significantly enhances hydroxyl (OH-) adsorption with insufficient OH- supply,thus improving HMF oxidation.To showcase the potential of Ru1-Co3O4 catalyst,we demonstrate its high efficiency in a flow reactor under industrially relevant conditions.Eventually,techno-economic analysis shows that substitution of the conventional1.0 mol L-1 KOH with 0.1 mol L-1 KOH electrolyte may significantly reduce the minimum selling price of FDCA by 21.0%.This work demonstrates an efficient catalyst design for electrooxidation of biomass working without using strong alkaline electrolyte that may contribute to more economic biomass electro-valorization.

【Abstract】 Electrocatalytic oxidation of 5-hydroxymethylfurfural (HMF) to 2,5-furandicarboxylic acid (FDCA),a sustainable strategy to produce bio-based plastic monomer,is always conducted in a high-concentration alkaline solution (1.0 mol L-1KOH) for high activity.However,such high concentration of alkali poses challenges including HMF degradation and high operation costs associated with product separation.Herein,we report a single-atom-ruthenium supported on Co3O4(Ru1-Co3O4) as a catalyst that works efficiently in a low-concentration alkaline electrolyte (0.1 mol L-1KOH),exhibiting a low potential of 1.191 V versus a reversible hydrogen electrode to achieve 10 m A cm-2 in 0.1 mol L-1 KOH,which outperforms previous catalysts.Electrochemical studies demonstrate that single-atom-Ru significantly enhances hydroxyl (OH-) adsorption with insufficient OH- supply,thus improving HMF oxidation.To showcase the potential of Ru1-Co3O4 catalyst,we demonstrate its high efficiency in a flow reactor under industrially relevant conditions.Eventually,techno-economic analysis shows that substitution of the conventional1.0 mol L-1 KOH with 0.1 mol L-1 KOH electrolyte may significantly reduce the minimum selling price of FDCA by 21.0%.This work demonstrates an efficient catalyst design for electrooxidation of biomass working without using strong alkaline electrolyte that may contribute to more economic biomass electro-valorization.

【基金】 supported by the National Key R&D Program of China (2023YFA1507400);Natural Science Foundation of Shandong Province (ZR2023QB094);Young Science and Technology, the National Natural Science Foundation of China (22325805 and 21935001);Beijing Natural Science Foundation (JQ22003)
  • 【文献出处】 Science Bulletin ,科学通报(英文) , 编辑部邮箱 ,2024年18期
  • 【分类号】TK6;TQ251.1;O643.36
  • 【下载频次】59
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