二氧化碳电催化还原中的电解质效应  

Designing Electrolytes for Aqueous Electrocatalytic CO_(2) Reduction

作　　者：荣佑文 桑佳琪 车丽 高敦峰 汪国雄[2] Youwen Rong;Jiaqi Sang;Li Che;Dunfeng Gao;Guoxiong Wang(School of Science,Dalian Maritime University,Dalian 116026,Liaoning Province,China;State Key Laboratory of Catalysis,Dalian National Laboratory for Clean Energy,Dalian Institute of Chemical Physics,Chinese Academy of Sciences,Dalian 116023,Liaoning Province,China;University of Chinese Academy of Sciences,Beijing 100049,China)

机构地区：[1]大连海事大学理学院,辽宁大连116026 [2]中国科学院大连化学物理研究所,催化基础国家重点实验室,辽宁大连116023 [3]中国科学院大学,北京100049

出　　处：《物理化学学报》2023年第5期93-110,共18页Acta Physico-Chimica Sinica

基　　金：国家重点研发计划(2021YFA1501503);国家自然科学基金(22002155,21973010,22125205,92045302);中科院战略性先导专项(XDA21061010);辽宁省兴辽英才计划(XLYC1907032);辽宁省自然科学基金(2021-MS-022);大连化物所创新基金(DICP I202203)资助项目。

摘　　要：二氧化碳(CO_(2))电催化还原反应利用可再生能源将CO_(2)转化为高值燃料和化学品,是一种新型的碳中和技术。CO_(2)电催化还原反应在电极/电解质界面上进行,因此除催化剂以外,电解质对提高CO_(2)电催化还原反应性能同样至关重要。本文深度剖析了CO_(2)电催化还原反应中的电解质效应,结合近几年的最新研究进展,详细讨论了局部pH、阳离子、阴离子和离子交换膜等电解质组成和性质对电催化活性和产物选择性的影响,阐述了电解质效应的催化作用机制。本文特别强调了电化学原位红外/拉曼等振动光谱在电解质效应机理研究方面的优势以及面向实际应用的膜电极CO_(2)电解器中阴离子、阳离子、水、液体产物等物质传输对活性、选择性、能量效率及CO_(2)利用效率等关键催化性能指标的影响。本文最后提出了当前电解质效应研究中存在的挑战,并展望了未来的研究机遇和发展趋势。As an emerging technology for achieving carbon neutrality,the electrocatalytic CO_(2)reduction reaction(CO_(2)RR)converts CO_(2)and water to valuable fuels and chemicals with power supply from renewable energy.Currently,the practical application of the CO_(2)RR suffers from insufficient electrocatalytic performance in terms of selectivity,reaction rate,energy efficiency,and long-term stability.Electrolytes are considered as equally critical as catalysts for enhancing the CO_(2)RR performance.From a catalysis perspective,electrolytes significantly affect the reaction microenvironments around catalytically active sites.From an electrochemical perspective,electrolytes determine the electric double layer structure.The electrocatalytic electrode/electrolyte interface where the CO_(2)RR takes place is strongly influenced by electrolyte composition and identity.Thus,beyond catalyst design,rational electrolyte design is an alternative strategy for advancing the CO_(2)RR towards industrial applications.This review presents important electrolyte effects in the aqueous CO_(2)RR using the most recent studies,with an emphasis on those conducted under industrially-relevant reaction conditions.The effects of(local)pH,cations,and anions in aqueous inorganic electrolytes and their coupled effects with solid polymer electrolytes on tuning the activity and selectivity of the CO_(2)RR are summarized.Although their influences on CO_(2)RR performance are interconnected,pH effects,cation effects,and anion effects as well as electrolyte effects in membrane electrode assembly(MEA)electrolyzers are discussed separately considering the leading role of each factor.The experimentally observed performance dependence on the electrolyte composition and identity as well as the underlying reaction mechanism are discussed.The unique role of vibrational spectroscopies,such as surface-enhanced infrared absorption and Raman,in the characterization of electrode/electrolyte interfaces and the elucidation of electrolyte effects is highlighted.An innovat

关 键 词：CO_(2)电催化还原 电解质效应 双电层 PH效应 阳离子效应 阴离子效应 固体聚合物电解质 膜电极 

分 类 号：O643[理学—物理化学]