石墨烯/CoSnO_(3)固载Pd-Pb纳米合金的制备及电催化氧化乙二醇  

Synthesis and electrocatalytic oxidation of ethylene glycol on Pd-Pb nanoalloys immobilized on graphene/CoSnO_(3) composites

作　　者：吴祉睿 马奇 王敏 莫晗 钟玉婷 刘红英[1] 周立群[1] WU Zhirui;MA Qi;WANG Min;MO Han;ZHONG Yuting;LIU Hongying;ZHOU Liqun(Collaborative Innovation Center for Advanced Organic Chemical Materials Co-constructed by the Province and Ministry,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)

机构地区：[1]有机化工新材料湖北省协同创新中心,有机功能分子合成与应用教育部重点实验室,湖北大学化学化工学院,湖北武汉430062

出　　处：《湖北大学学报（自然科学版）》2022年第3期277-286,共10页Journal of Hubei University：Natural Science

基　　金：有机功能分子合成与应用教育部重点实验室项目(KLSAOFM1913)资助。

摘　　要：本工作采用水热-煅烧法合成出载体GO/CoSnO_(3),再通过浸渍还原法将Pd、PdPb纳米粒子(NPs)负载到载体上,制备出Pd@rGO/CoSnO_(3)、PdPb@rGO/CoSnO_(3)新型阳极电催化剂,并用于碱性介质中乙二醇(EG)的电催化氧化.采用多种测试手段对产物的结构、组成及价态进行分析.结果表明,当摩尔比Pd∶Pb=1∶0.2时,Pd_(1)Pb_(0.2)@rGO/CoSnO_(3)催化剂的正向峰电流密度高达205.41 mA·cm^(-2),是单金属催化剂Pd@rGO/CoSnO_(3)(136.39 mA·cm^(-2))的1.5倍,更是商业Pd/C(27.1 mA·cm^(-2))的7.5倍,具有最佳的电催化活性、稳定性和抗毒性.这种杰出的电催化活性主要归因于GO/CoSnO_(3)复合载体具有立方体结构以及丰富的含氧原子,有利于金属的均匀负载;同时,Pd和Pb之间存在着强烈的电子效应以及提供丰富的含氧物种,从而显著提升了电催化活性和稳定性,这为乙二醇燃料电池电催化剂的开发提供了重要参考.The carrier GO/CoSnO_(3) was synthesized by hydrothermal-calcination method,then Pd and PdPb NPs were successfully fixed on the carrier by impregnation reduction route to get the novel anode electrocatalysts Pd@rGO/CoSnO_(3) and PdPb@rGO/CoSnO_(3),which were used to the electrocatalytic oxidation of EG in alkaline medium.The structure,component and valence state of the product were characterized through various techniques.The result shows that,when the molar ratio Pd∶Pb=1∶0.2,the forward peak current density of bimetallic catalyst Pd_(1)Pb_(0.2)@rGO/CoSnO_(3) is as high as 205.41 mA·cm^(-2),which is 1.5 times of the Pd@rGO/CoSnO_(3)(136.39 mA·cm^(-2)),and 7.5 times of commercial Pd/C(27.1 mA·cm^(-2)).Compared with the Pd@rGO/CoSnO_(3),Pd_(1)Pb_(0.1)@rGO/CoSnO_(3) and Pd_(1)Pb_(0.3)@rGO/CoSnO_(3),the Pd_(1)Pb_(0.2)@rGO/CoSnO_(3) exhibits the highest electrocatalytic activity,stability and anti-toxicity.The excellent electrocatalytic performance is attributed to the unique cube GO/CoSnO_(3) and rich oxygen atoms of surface for the bimetallic PdPb loading uniformly.Meanwhile,the strong electronic effect between Pd and Pb can provide abundant oxygen-containing species,which significantly enhances the electrocatalytic activity and stability for EG oxidation.It will provide an important reference for developing advanced eletrocatalysts in direct EG fuel cells.

关 键 词：石墨烯 CoSnO_(3) Pd-Pb纳米合金 电催化氧化 乙二醇 

分 类 号：O643.3[理学—物理化学]