自支撑BiCu/碳杂化纳米纤维膜高效促进CO2电还原生成甲酸
Self-supporting BiCu/carbon hybrid nanofiber membrane promotes efficient CO2 electroreduction to formate
宋德文 1张世鹏 1宁汇 1费翔 1汪明旺 1王小珊 1吴文婷 1赵青山 1李永哲 2吴明铂1
作者信息
- 1. State Key Laboratory of Heavy Oil Processing,College of Chemical Engineering,College of New Energy,Institute of New Energy,China University of Petroleum(East China),Qingdao 266580,China
- 2. Shandong Dongyue Future Hydrogen Energy Material Co.,Ltd,Zibo 256412,China
- 折叠
摘要
二氧化碳电还原有利于二氧化碳高价值利用和间歇性电能的存储,是一种极具应用前景的新技术.自支撑催化剂比粉末催化剂在构建电极方面具有明显优势,但缺乏有效的合成方法.本研究采用电纺丝-碳化法合成了一种自支撑的BiCu/碳杂化纳米纤维膜(BiCu/CHNM),可直接用作工作电极在流动池中将二氧化碳还原为甲酸盐,其法拉第效率为87.67％,分电流密度为142.9 mA cm-2.稳定性测试中,甲酸盐的法拉第效率在高偏电流密度(＞100 mA cm-2)下可在50小时内连续保持在80％以上.原位拉曼光谱和密度泛函理论计算证实,铜掺杂降低了Bi(012)平面上HCOO-形成的能垒,同时提高了碳纳米纤维网络的导电性.由于同时具有高导电框架结构和高度分散的BiCu活性位点,这种杂化膜同时表现出高活性、高选择性和长时间稳定性.
Abstract
CO2 electroreduction is an alluring technology for high-value CO2 utilization and intermittent electrical en-ergy storage.Self-supporting catalysts with high efficiency have clear advantages over powder ones in electrode con-struction but still lack effective synthesis methods.In this work,a self-supporting BiCu/carbon hybrid nanofiber mem-brane(BiCu/CHNM)was synthesized by electrospinning-cal-cination and employed directly as a working electrode in a flow cell for CO2 electroreduction to formate with a high Faradaic efficiency of 87.67％at a partial current density of 142.9 mA cm-2.In stability tests,the Faradaic efficiency of formate remained at 80％for 50 h at high partial current densities(＞100 mA cm-2).In-situ Raman spectra and density functional theory calculations confirmed that copper doping lowers the energy barrier of HCOO-formation on the Bi(012)plane and increases the conductivity of the carbon nanofiber network.Due to the well-designed conductive framework and the highly dispersed BiCu active sites,this hybrid membrane shows high activity,high selectivity,and long stability si-multaneously.
关键词
carbon dioxide/self-supporting catalyst/composite catalyst/electroreductionKey words
carbon dioxide/self-supporting catalyst/composite catalyst/electroreduction引用本文复制引用
基金项目
国家自然科学基金(52072409)
Major Scientific and Technological Innovation Project of Shandong Province(2020CXGC010403)
Taishan Scholar Project of Shandong Province of China(ts201712020)
出版年
2024
NETL
NSTL
万方数据