摘要
探究分子簇可控热解过程是研究分子簇热解后产物的微观结构与其电催化活性之间的关系的有效途径,然而开发具有高活性位点和优化内在活性的析氧反应(OER)/尿素氧化反应(UOR)双功能电催化剂依旧是一个很大的挑战。因此,我们引入了1,3-二氨基-2-丙醇缩3-甲氧基水杨醛席夫碱HL配体合成的四核镍钴基配合物作为前驱体,在氮气气氛下进行低温热解后制备得到了双金属掺杂的Ni_(2)Co_(2)-T材料,并作为OER/UOR双功能电催化剂。双金属原子与配位溶剂之间的配位模式,暴露出了更多的活性中心,为提高催化活性提供了更多的可能。在1.0 mol/L KOH溶液中,配合物Ni_(2)Co_(2)-350的过电位仅需232 mV就能达到10 mA·cm^(-2)的基准电流密度,在1.0 mol/L KOH+0.33 mol/L Urea溶液中电势为1.367 V,并且均表现出良好的稳定性,具有优异的OER/UOR性能。该工作中分子簇热解机理的研究对于未来实现多功能电催化具有重要意义。
Exploring the controlled pyrolysis process of molecular clusters is an effective way to study the relationship between the microstructure of the products after pyrolysis of molecular clusters and their electrocatalytic activity.However,it is still a great challenge to develop bifunctional electrocatalysts with high active sites and optimized intrinsic activity of oxygen evolution reaction(OER)/urea oxidation reaction(UOR).Therefore,we introduced a tetranuclear nickel-cobalt complex synthesized by 1,3-diamino-2-propyl alcohol 3-methoxysalicylaldehyde Schiff base HL ligand as a precursor.Bimetallic doped Ni_(2)Co_(2)-T material was prepared by low temperature pyrolysis in a nitrogen atmosphere and used as an OER/UOR bifunctional electrocatalyst.The coordination pattern between bimetallic atoms and the coordination solvent exposed more active centers and provided more possibilities for improving catalytic activity.In 1.0 mol/L KOH solution,the overpotential of the complex Ni_(2)Co_(2)-350 only needed 232 mV to reach the reference current density of 10 mA·cm^(-2),and in 1.0 mol/L KOH+0.33 mol/L Urea solution,the potential was 1.367 V.All of them show good stability and have excellent OER/UOR performance.The study of the mechanism of molecular cluster pyrolysis in this work is of great significance for the realization of multifunctional electrocatalysis in the future.
作者
甘梅杏
王璐
周芳蕾
彭旭
GAN Meixing;WANG Lu;ZHOU Fanglei;PENG Xu(Hubei Collaborative Innovation Center for Advanced Organic Chemical Materials,Ministry of Education Key Laboratory for the Synthesis and Application of Organic Functional Molecules,College of Chemistry and Chemical Engineering,Hubei University,Wuhan 430062,China)
出处
《湖北大学学报(自然科学版)》
2025年第2期239-246,共8页
Journal of Hubei University:Natural Science
基金
武汉市知识创新专项(2023020201020422)资助。
关键词
电催化
低温热解
协同效应
电解水产氧
双功能电催化剂
coordination molecular clusters
low-temperature pyrolysis
synergistic effect
water splitting
bifunctional electrocatalyst
