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作 者:吴进 刘京 夏雾 任颖异 王锋 Jin Wu;Jing Liu;Wu Xia;Ying-Yi Ren;Feng Wang(Key Laboratory of Materials Chemistry for Energy Conversion and Storage(Huazhong University of Science and Technology)of Ministry of Education,Hubei Key Laboratory of Material Chemistry and Service Failure,School of Chemistry and Chemical Engineering,Huazhong University of Science and Technology,Wuhan 430074,China)
机构地区:[1]材料化学与服役失效湖北省重点实验室,能量转化与存储材料化学教育部重点实验室(华中科技大学),华中科技大学化学与化工学院,武汉430074
出 处:《物理化学学报》2021年第5期95-102,共8页Acta Physico-Chimica Sinica
基 金:国家自然科学基金(21871102);中央高校基本科研业务费专项资金(2019kfyRCPY101)资助项目。
摘 要:二氧化碳(CO_(2))是大气层中温室气体的主要成分,资源化利用二氧化碳既可以减少二氧化碳排放又可以利用二氧化碳制备高附加值化学品。通过人工光合作用系统将二氧化碳还原为一氧化碳、甲烷等太阳燃料被认为是二氧化碳资源化利用的理想方式。纳米半导体材料因其丰富的光物理和光化学特性以及优异的光稳定性被作为光敏剂或光催化剂用于构筑光催化二氧化碳还原体系,其中CdS和CdSe(如溶胶量子点、纳米棒、纳米片)是研究较多的两种纳米半导体材料。基于CdS或CdSe纳米半导体材料的光催化二氧化碳还原体系可分为三类:(i)基于CdS、CdSe的光催化二氧化碳还原体系;(ii)基于CdS、CdSe复合材料的二氧化碳还原体系;(iii)CdS和分子催化剂构筑的杂化二氧化碳还原体系。本文介绍了人工光合作用体系的构筑以及半导体纳米材料光催化机理,总结了上述三类体系中的代表性工作,最后讨论了基于纳米半导体材料的光催化二氧化碳还原研究前景和面临的挑战。Carbon dioxide(CO_(2))is one of the main greenhouse gases in the atmosphere.The conversion of CO_(2)into solar fuels(CO,HCOOH,CH4,CH3OH,etc.)using artificial photosynthetic systems is an ideal way to utilize CO_(2)as a resource and reduce CO_(2)emissions.A typical artificial photosynthetic system is composed of three key components:a photosensitize r(PS)to harvest visible light,a catalyst(C)to catalyze CO_(2)or protons into carbon-based fuels or H2,respectively,and a sacrificial electron donor(SED)to consume the holes generated in the PS.In most cases,the PS and catalyst are two different components of a system.However,some components that possess both light harvesting and redox catalysis functionalities,e.g.,nano-semiconductors,are referred to as photocatalysts.During photocatalysis,the PS is typically excited by photons to generate excited electrons.The excited electrons in the PS are transferred to the catalyst to generate a reduced catalyst.The reduced catalyst is used as an active intermediate to perform CO_(2)binding and transformation.The PS can be recovered through a reaction with the SED.Nano-semiconductors have been used as photosensitizers and/or photocatalysts in photocatalytic CO_(2)reduction systems owing to their excellent photophysical and photochemical properties and photostability.CdS and CdSe nano-semiconductors,such as quantum dots,nanorods,and nanosheets,have been widely used in the construction of photocatalytic CO_(2)reduction systems.Systems based on CdS or CdSe nano-semiconductors can be classified into three categories.The first category is systems based on CdS or CdSe photocatalysts.In these systems,CdS or CdSe nano-semiconductors function as photocatalysts to catalyze CO_(2)reduction without a co-catalyst under visible-light irradiation.The CO_(2)reduction reaction occurs at the surface of the CdS or CdSe nano-semiconductors.The second category is systems based on CdS or CdSe composite photocatalysts.CdS or CdSe nano-semiconductors are combined with functional materials,such as reduced
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