铜业工程:2023(1):1-11
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三维自支撑的铜铋双金属电沉积制备及其电催化还原CO2性能研究
陈嘉磊, 廖雪龙, 陈山, 卢天天, 孙潇婷, 曹丽馨, 王欢
(南开大学化学学院)
Self-Supported CuBi Bimetal Nanodendrites for CO2 Electrochemical Reduction
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本文已被:浏览 7195次   下载 10153
投稿时间:2023-01-03    修订日期:2023-01-17
中文摘要: 金属铜(Cu)是二氧化碳(CO2)还原为甲酸的常见催化剂,但是存在竞争析氢副反应(HER)严重和稳定性差等问题。引入第二金属的合金化策略可以有效改善上述问题,但是复杂的合成方法限制了电催化CO2还原技术中的实际应用。鉴于此,开发了一种简单、快速、低能耗的原电池沉积法,以还原电势差为反应驱动力,通过调节前驱体浓度在石墨烯基底上原位生长具有三维自支撑结构的铜铋(CuBi)双金属纳米枝晶(nCuBi-G/Cufoil)。研究表明:nCuBi-G/Cufoil结构中Bi作为电子供体向Cu提供电子,从而增加Cu中心电子密度,可以有效抑制CO2RR过程中的析氢反应,大幅提高甲酸产物的选择性,并且降低了电极表面的积碳浓度,提高CO2电催化反应的稳定性。此外,石墨烯导电基底可以加速CuBi和基底之间电子传递过程,改善CO2催化过程动力学,提高CO2RR活性。基于以上效应,nCuBi-G/Cufoil表现出95.9%的甲酸选择性,并且在此电压下可以稳定运行20h,且甲酸选择性保持在90%以上。本文为实现高效制备双金属催化剂提供了绿色合成策略,并揭示了金属电子结构和导电基底对CO2电催化性能的影响。
Abstract:Copper(Cu)have been extensively studied for electrochemical conversion of carbon dioxide(CO2)into formate,but have a series of problem such as the competing hydrogen evolution reaction (HER)and poor stability. The introduction of another metal into metallic Cu to construct Cu-based alloy has shown great promise in alleviating the problem. However,the complicated synthetic routes severely restrict their practical applications. Herein,this paper reported the galvanic-cell deposition for the rapid synthesis of self-supported CuBi nanodendrites directly grown on graphene covered Cu foil(nCuBi-G/Cu foil). The host metal Bi could donor electron from Bi to Cu,which enabled superior CO2 reduction performance. nCuBi-G/Cu foil achieved a formate Faradaic efficiency of 95.91% at -0.93 V(vs. RHE)and delivers a stable current density of about 20.1 mA/cm2 with a negligible decay during 20 h of continuous electrocatalysis. Furthermore,it was found that graphene as deposition substrate could accelerate electron transfer,contributing to an excellent activity of CO2 reduction This work provided a novel strategy for the green synthesis of efficient CuBi bimetal catalysts for CO2 reduction and demonstrated the substrate and electronic engineering strategy to improve the CO2 reduction activity.
文章编号:20230103001     中图分类号:TF813; TF804.2
基金项目:国家自然科学基金项目(22105107)
引用文本: 陈嘉磊,廖雪龙,陈山,卢天天,孙潇婷,曹丽馨,王欢.三维自支撑的铜铋双金属电沉积制备及其电催化还原CO2性能研究[J].铜业工程,2023,(1):1-11