物理化学学报 >> 2022, Vol. 38 >> Issue (12): 2201050.doi: 10.3866/PKU.WHXB202201050

所属专题： 纪念傅鹰先生诞辰120周年

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PtRuAgCoNi高熵合金纳米颗粒高效电催化氧化5-羟甲基糠醛

杨艳1, 何博文1, 马华隆1, 杨森2, 任州宏1, 秦天1, 卢发贵1, 任力闻2, 张熠霄1, 王天富2,*(), 刘晰1,*(), 陈立桅1,*()   

  1. 1 上海交通大学化学化工学院, 物质科学原位中心, 转化分子前沿科学中心, 上海 200240
    2 上海交通大学环境科学与工程学院, 上海 200240
  • 收稿日期:2022-01-29 录用日期:2022-03-15 发布日期:2022-03-21
  • 通讯作者: 王天富,刘晰,陈立桅 E-mail:tfwang@sjtu.edu.cn;liuxi@sjtu.edu.cn;lwchen2018@sjtu.edu.cn
  • 基金资助:
    国家重点研发计划(2021YFA1500300);国家重点研发计划(2021YFA1500303);国家重点研发计划(2021YFB3800300);国家自然科学基金(21991153);国家自然科学基金(21991150);国家自然科学基金(22072090)

PtRuAgCoNi High-Entropy Alloy Nanoparticles for High-Efficiency Electrocatalytic Oxidation of 5-Hydroxymethylfurfural

Yan Yang1, Bowen He1, Hualong Ma1, Sen Yang2, Zhouhong Ren1, Tian Qin1, Fagui Lu1, Liwen Ren2, Yixiao Zhang1, Tianfu Wang2,*(), Xi Liu1,*(), Liwei Chen1,*()   

  1. 1 School of Chemistry and Chemical Engineering, In-situ Center for Physical Sciences, Frontiers Science Center for Transformative Molecules, Shanghai Jiao Tong University, Shanghai 200240, China
    2 School of Environmental Science and Engineering, Shanghai Jiao Tong University, Shanghai 200240, China
  • Received:2022-01-29 Accepted:2022-03-15 Published:2022-03-21
  • Contact: Tianfu Wang,Xi Liu,Liwei Chen E-mail:tfwang@sjtu.edu.cn;liuxi@sjtu.edu.cn;lwchen2018@sjtu.edu.cn
  • About author:Email: lwchen2018@sjtu.edu.cn (L.C.)
    Email: liuxi@sjtu.edu.cn (X.L.)
    Email: tfwang@sjtu.edu.cn (T.W.)
  • Supported by:
    the National Key R & D Plan(2021YFA1500300);the National Key R & D Plan(2021YFA1500303);the National Key R & D Plan(2021YFB3800300);the National Natural Science Foundation of China(21991153);the National Natural Science Foundation of China(21991150);the National Natural Science Foundation of China(22072090)

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摘要：

5-羟甲基糠醛(HMF)的电催化氧化被认为是合成2,5-呋喃二甲酸(FDCA)最环保、经济和有效的方法之一，它可作为聚呋喃二甲酸乙二醇酯(PEF)的生物基前体。在这项工作中，我们通过低温溶剂热法合成了PtRuAgCoNi高熵合金纳米颗粒，并在不改变颗粒结构和组成的情况下进行了简易的处理以去除表面活性剂。负载在碳载体上的合金纳米催化剂无论是否含有表面活性剂在HMF电催化氧化为FDCA的过程中都表现出比商业Pt/C更好的催化性能。且表面活性剂的去除可以进一步提高其电催化性能，表明高熵合金纳米粒子在电催化和绿色化学中具有广阔的应用前景。

关键词: 高熵合金, 表面活性剂, 溶剂热合成, 电催化氧化, 5-羟甲基糠醛, 2,5-呋喃二甲酸

Abstract:

Electrocatalytic oxidation of 5-hydroxymethylfurfural (HMF) is considered one of the most environment friendly, economical, and efficient methods for synthesizing 2,5-furandicarboxylic acid (FDCA), which is a promising bio-based precursor of polyethylene 2,5-furandicarboxylate. In this study, we synthesized PtRuAgCoNi high-entropy alloy nanoparticles, with an average diameter of approximately 9 nm, using a solvothermal method. The synthesized nanoparticles displayed a core-shell microstructure, in which Co, Ru, Ag, and Ni were distributed over the entire core-shell microstructure of each nanoparticle, while Pt was mainly concentrated in the shell structure. A two-step method, including small-molecule substitution and low-temperature calcination, was used to remove the surfactant from the synthesized nanoparticles without changing the structure and composition of the nanoparticles. After being deposited on a carbon support, the high-entropy alloy nanoparticles, with or without surfactants, exhibited better catalytic performance in the electrocatalytic oxidation of HMF to FDCA than the commercial Pt/C catalyst. The removal of surfactants after calcination at 185 ℃ can further improve electrocatalytic performance, suggesting promising application prospects of high-entropy alloy nanoparticles in electrocatalysis and green chemistry.

Key words: High entropy alloy, Surfactant, Solvothermal synthesis, Electrocatalytic oxidation, 5-Hydroxymethylfurfural, 2,5-Furandicarboxylic acid