首页|酸性流动电解槽中电催化还原CO2制CO的界面优化及工艺放大研究

酸性流动电解槽中电催化还原CO2制CO的界面优化及工艺放大研究

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基于可再生能源的电催化二氧化碳还原反应(eCO2RR)可以将CO2转化为高附加值的化学品和燃料,是应对大气CO2浓度急剧升高和全球变暖的一种可行方案。然而,在传统的中性或碱性电解液中,eCO2RR存在严重的碳损失问题,导致CO2的理论单程碳转化率(SPCE)低于50%,同时电解液的再生需要消耗额外能源。相比之下,酸性电解液可以有效解决碳损失问题,其理论SPCE可达100%,备受研究者关注。目前大多数研究仍集中在催化剂的优化上,而对气体扩散电极(GDE)、电解质和质子膜等固液气界面的优化关注不足,这些因素均会影响eCO2RR的选择性、稳定性和能量效率。通过系统优化酸性eCO2RR三相界面(固相、液相、气相),在100 mA,cm-2电流密度和低于5 V的槽压下,实现了法拉第效率(FECO)超过90%,并且稳定运行110h。最后,将电极面积放大至100 cm2,初步研究了工艺放大的影响机制,并提出了一种新的间歇运行策略。针对酸性eCO2RR的界面优化和工艺放大研究有望为其工业化应用提供理论支持。
Interface optimization and process scale-up study of electrocatalytic reduction of CO2 to CO in acidic flow electrolyzers
The electrocatalytic carbon dioxide reduction reaction(eCO2RR)powered by renewable energy can convert CO2 into high-value chemicals and fuels.It is a viable solution to address the sharp increase in atmospheric CO2 concentration and global warming.However,in traditional neutral or alkaline electrolytes,eCO2RR suffers from severe carbon loss,resulting in a theoretical single-pass carbon conversion efficiency(SPCE)of less than 50%,and the regeneration of the electrolyte requires additional energy.Acidic electrolytes can effectively solve the carbon loss issue,achieving a theoretical SPCE of 100%,which has attracted widespread attention worldwide.Nevertheless,most previous studies focused on catalyst optimization,with insufficient emphasis on optimizing solid-liquid-gas interfaces such as gas diffusion electrodes(GDEs),electrolytes,and proton membranes.These factors influence the selectivity,stability,and energy efficiency of eCO2RR.In this study,we systematically optimized the three-phase interface(solid,liquid,and gas)of the acidic eCO2RR,achieving a faradaic efficiency for CO(FECO)of over 90%at a current density of 100 mA·cm-2 and a cell voltage of less than 5 V,with stable operation for 110 hours.Finally,we scaled up the electrode area to 100 cm2,exploring the impact mechanism of process scale-up,and proposing a new intermittent operation strategy.This research on interface optimization and process scale-up of acidic eCO2RR is expected to provide a theoretical foundation for its potential industrial applications.

Acidic electrolyteFlow electrolyzerCO2COElectrocatalysisInterface optimization

马飞余、卢先龙、赵学洋、王丽丽、李振东、邓邦为、董帆

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中国气象局气候资源经济转化重点开放实验室,重庆 401147

电子科技大学长三角研究院(湖州),浙江湖州 313001

浙江工业大学环境学院,浙江 杭州 310014

西南交通大学环境科学与工程学院,四川成都 611756

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酸性电解液 流动电解槽 CO2 CO 电催化 界面优化

2024

能源环境保护
煤炭科学研究总院杭州环境保护研究所

能源环境保护

影响因子:0.472
ISSN:1006-8759
年,卷(期):2024.38(6)