咪唑鎓盐基材料电催化二氧化碳还原研究进展OA北大核心CSTPCD
Imidazolium-Based Materials for CO2 Electroreduction
随着化石能源的使用日益增加,大气中CO2的浓度不断上升,给环境带来了挑战.通过催化将CO2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CO2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CO2电还原反应(CO2RR)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CO2RR的有潜力的候选材料.这些材料对CO2有很强的亲和力,并且在CO2RR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CO2,有效地抑制析氢副反应(HER),并提高CO2RR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CO2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CO2RR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CO2RR.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CO2RR中的性能有影响.N-杂环卡宾(NHC)基电催化剂作为咪唑鎓与CO2相互作用的活性形式之一,表现出优异的CO2RR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CO2的能力,从而提高CO2RR活性.总之,在CO2RR中使用咪唑鎓基材料对于推进CO2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 CO2 in the atmosphere is rising,leading to environmental challenges.However,the conversion of CO2 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 CO2 emissions and achieve carbon neutrality.Among various methods,the CO2 electroreduction reaction(CO2RR)using renewable clean energy has garnered significant attention due to its mild reaction conditions,controlled reactions progress,environmental friendliness,and numerous value-added products it can yield.In this context,imidazolium-based materials and their derivatives have emerged as promising candidates for CO2RR.These materials have a strong affinity for CO2 and find applications as both electrolytes and electrocatalysts in CO2RR systems.So one of their key advantages,especially Im-ILs,is their ability to enrich CO2 in catalytic systems,effectively preventing the undesired hydrogen evolution reaction(HER)and enhancing the selectivity towards CO2RR products.Understanding the interaction mechanism between imidazolium-based ionic liquids(Im-ILs)and CO2 molecules under electrocatalytic conditions is crucial for gaining deeper insights into why the addition of Im-ILs can improve CO2RR 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 CO2RR.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 CO2RR.Lastly,N-heterocyclic carbene(NHC)-based electrocatalysts,as one of the active forms of imidazolium interaction with CO2,have demonstrated exceptional performance.When introduced into porous heterogeneous catalysts and molecular catalysts,NHC-based electrocatalysts stabilize metal nanoparticles and enhance the ability to capture CO2,thus promoting CO2RR activity.In summary,the utilization of imidazolium-based materials in CO2RR holds great promise for advancing the field of CO2 conversion and achieving more sustainable and efficient processes for high-value chemical synthesis.
张强;黄远标;曹荣
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||中国科学技术大学化学与材料科学学院化学系,合肥 230000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||中国福建光电信息科学与技术创新实验室,福州 350108||中国科学院大学,北京 100049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||中国福建光电信息科学与技术创新实验室,福州 350108||中国科学技术大学化学与材料科学学院化学系,合肥 230000||中国科学院大学,北京 100049
化学
CO2电还原离子液体咪唑鎓盐氮杂环卡宾金属纳米颗粒
CO2 electroreductionIonic liquidsImidazoliumN-heterocyclic carbeneMetal nanoparticles
《物理化学学报》 2024 (004)
光活性基元构筑的氢键有机框架化合物及其药物传输和光动力协同治疗性能
131-145 / 15
This project was supported by the National Key Research and Development Program of China(2018YFA0704502),the National Natural Science Foundation of China(U22A20436,2071245,22033008,22220102005),and the Fujian Science&Technology Innovation Laboratory for Optoelectronic Information of China(2021ZZ103).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
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