巯基配位的金属有机框架在高效电催化析氧中的应用  

Metal-Organic Frameworks with Sulfhydryl Coordination for Efficient Electrocatalytic Oxygen Evolution Reaction

作　　者：郑炜琼 刘习奎[1] 李爽 程冲[1] Weiqiong Zheng;Xikui Liu;Shuang Li;Chong Cheng(State Key Laboratory of Polymer Materials Engineering,Polymer Research Institute of Sichuan University,Chengdu 610065,China)

机构地区：[1]四川大学高分子科学与工程学院高分子材料工程国家重点实验室,四川成都610065

出　　处：《高分子材料科学与工程》2024年第6期106-114,共9页Polymer Materials Science & Engineering

基　　金：国家自然科学基金资助项目(52273269)。

摘　　要：金属有机框架(MOFs)材料已被探索作为析氧反应(OER)的有效电催化剂。然而,在大电流密度下,MOFs结构不稳定的问题严重阻碍了其大规模应用。文中采用硫醇官能化的2,5-二巯基对苯二甲酸(H4DMBD)与FeNi金属离子配合制备了一种具有巯基S配位的双金属MOFs(FeNi-DMBDC)。得益于独特的Fe-S和Ni-S配位结构,FeNi-DSBDC在碱性OER催化中表现出高活性和良好的稳定性,只需要274 mV的过电位就可达到100 mA/cm2的工作电流密度。同时,负载在导电载体碳布(CC)上的FeNi-DSBDC可以实现安培级的工作电流密度,在50mA/cm2和100mA/cm2的电流密度下具有长期稳定性(>200 h)。这不仅拓宽了MOFs材料在高效稳定的OER催化剂中的应用潜力,也为分子设计和配体调控策略在催化剂设计中的作用提供了新见解。Metal-organic frameworks(MOFs)materials have been explored as effective electrocatalysts for oxygen evolution reaction(OER).However,their structural instability at high current densities has hindered their large-scale industrial application.Herein,S-coordinated bimetallic MOFs(FeNi-DMBDC)were synthesized by the thiol-functionalized 2,5-dimercaptoterephthalic acid(H4DMBD)with FeNi metal ion coordination.Benefit from the unique Fe-S and Ni-S coordination structures,the FeNi-DSBDC exhibits high activity and good stability in alkaline OER catalysis,which requires a low overpotential of only 274 mV to reach the current density of 100 mA/cm2.Meanwhile,when FeNi-DSBDC was loaded on a conductive carrier carbon cloth(CC),it can achieve amperometry current densities and operate stably for more than 200 h at the current densities of 50 mA/cm2 and 100 mA/cm2.This study not only broadened the potential of MOFs materials for efficient and stable anodic catalysis,but also provided new insights into the role of utilizing molecular design and ligand modulation strategies in electrocatalyst design.

关 键 词：金属有机框架 析氧反应 电催化剂 配位调控 

分 类 号：O641.4[理学—物理化学]