咪唑鎓盐基材料电催化二氧化碳还原研究进展  

Imidazolium-Based Materials for CO_(2) Electroreduction

作　　者：张强 黄远标[1,2,4] 曹荣 Qiang Zhang;Yuanbiao Huang;Rong Cao(State Key Laboratory of Structural Chemistry,Fujian Institute of Research on the Structure of Matter,Chinese Academy of Sciences,Fuzhou 350002,China;Fujian Science&Technology Innovation Laboratory for Optoelectronic Information of China,Fuzhou 350108,China;Department of Chemistry,School of Chemistry and Materials Science,University of Science and Technology of China,Hefei,230000,China;University of Chinese Academy of Sciences,Beijing 100049,China)

机构地区：[1]中国科学院福建物质结构研究所,结构化学国家重点实验室,福州350002 [2]中国福建光电信息科学与技术创新实验室,福州350108 [3]中国科学技术大学化学与材料科学学院化学系,合肥230000 [4]中国科学院大学,北京100049

出　　处：《物理化学学报》2024年第4期131-145,共15页Acta Physico-Chimica Sinica

基　　金：国家重点研发计划(2018YFA0704502);国家自然科学基金(U22A20436,2071245,22033008,22220102005);福建省光电信息科技创新实验室(2021ZZ103)资助项目。

摘　　要：随着化石能源的使用日益增加,大气中CO_(2)的浓度不断上升,给环境带来了挑战。通过催化将CO_(2)转化为高附加值化学品为解决这些问题提供了一个机会,并为燃料合成开辟了一条新的途径,最终有助于减少CO_(2)排放并实现碳中和。在众多的方法中,利用可再生清洁能源进行CO_(2)电还原反应(CO_(2)RR)以其反应条件温和、反应进度可控、环境友好以及可以产生大量的附加值产品而受到重视。在此背景下,咪唑鎓基材料及其衍生物已成为CO_(2)RR的有潜力的候选材料。这些材料对CO_(2)有很强的亲和力,并且在CO_(2)RR系统中作为电解质和电催化剂都有应用。所以它们的主要优点之一是能够在催化体系中富集CO_(2),有效地抑制析氢副反应(HER),并提高CO_(2)RR产物的选择性。了解电催化条件下咪唑鎓基离子液体(Im-ILs)与CO_(2)分子之间的相互作用机制对于从分子角度深入了解为什么添加Im-ILs可以改善CO_(2)RR性能至关重要。此外在非均相电催化剂中,Im-ILs作为表面修饰基团和捕集剂,可以显著改变催化剂的表面环境和疏水性,从而促进CO_(2)RR。值得注意的是,Lehn型和金属卟啉分子催化剂中的咪唑鎓基团已被发现对这些催化剂在CO_(2)RR中的性能有影响。N-杂环卡宾(NHC)基电催化剂作为咪唑鎓与CO_(2)相互作用的活性形式之一,表现出优异的CO_(2)RR性能。将NHC基电催化剂引入多孔多相催化剂和分子催化剂中,可以稳定金属纳米颗粒,提高捕获CO_(2)的能力,从而提高CO_(2)RR活性。总之,在CO_(2)RR中使用咪唑鎓基材料对于推进CO_(2)转化,实现可持续、有效合成高附加值化学品具有巨大的前景。With the increasing use of fossil energy sources,the concentration of CO_(2) in the atmosphere is rising,leading to environmental challenges.However,the conversion of CO_(2) into high value-added chemicals through catalysis presents an opportunity to address these issues and create a new pathway for fuel synthesis,ultimately helping to reduce CO_(2) emissions and achieve carbon neutrality.Among various methods,the CO_(2) electroreduction reaction(CO_(2)RR)using renewable clean energy has garnered significant attention due to its mild reaction conditions,controlled reactions progress,environmental friendliness,and numerous valueadded products it can yield.In this context,imidazolium-based materials and their derivatives have emerged as promising candidates for CO_(2)RR.These materials have a strong affinity for CO_(2) and find applications as both electrolytes and electrocatalysts in CO_(2)RR systems.So one of their key advantages,especially Im-ILs,is their ability to enrich CO_(2) in catalytic systems,effectively preventing the undesired hydrogen evolution reaction(HER)and enhancing the selectivity towards CO_(2)RR products.Understanding the interaction mechanism between imidazolium-based ionic liquids(Im-ILs)and CO_(2) molecules under electrocatalytic conditions is crucial for gaining deeper insights into why the addition of Im-ILs can improve CO_(2)RR performance from a molecular perspective.Furthermore,Im-ILs can serve as both surface modifier groups and trapping agents in heterogeneous electrocatalysts,which can significantly alter the surface environment and hydrophobicity of the catalysts,leading to improved CO_(2)RR.Notably,the imidazolium groups present in Lehn-type and metal-porphyrin molecular catalysts have been found to have an impact on the performance of these catalysts in CO_(2)RR.Lastly,N-heterocyclic carbene(NHC)-based electrocatalysts,as one of the active forms of imidazolium interaction with CO_(2),have demonstrated exceptional performance.When introduced into porous heterogeneous catalysts and

关 键 词：CO_(2)电还原 离子液体 咪唑鎓盐 氮杂环卡宾 金属纳米颗粒 

分 类 号：O646[理学—物理化学]