金属纳米团簇修饰的g-C_(3)N_(4)在光催化中的最新进展  

Recent advances in metal nanocluster-modified g-C_(3)N_(4)for photocatalysis

作　　者：李宇涵[1] 宋欣源 欧阳平[1] 段有雨 董帆[1] Yuhan Li;Xinyuan Song;Ping Ouyang;Youyu Duan;Fan Dong(Chongqing Key Laboratory of Catalysis and New Environmental Materials,School of Environment and Resources,Engineering Research Center for Waste Oil Recovery Technology and Equipment,Ministry of Education,Chongqing Technology and Business University,Chongqing 400067,China;Chongqing Institute of New Energy Storage Materials and Equipment,Chongqing University,Chongqing 400044,China)

机构地区：[1]重庆工商大学废油资源化技术与装备教育部工程研究中心,环境与资源学院,重庆市催化与环境新材料重点实验室,重庆400067 [2]重庆大学,重庆新型储能材料与装备研究院,重庆400044

出　　处：《科学通报》2024年第21期3130-3143,共14页Chinese Science Bulletin

基　　金：国家自然科学基金(52370109,51808080);重庆市留学人员回国创业创新支持重点计划(cx2022005);重庆市基础研究与前沿探索项目(CSTB2022NSCQ-MSX0035,CSTB2023NSCQ-LZX0096);重庆市教委科学技术研究计划(KJQN201800826,KJZDK201800801,KJZDM202300802);中国博士后科学基金面上资助(2022M710830);校内高层次人才引进项目(1856039)资助。

摘　　要：石墨相氮化碳(graphitic carbon nitride,g-C_(3)N_(4))作为一种不含金属的聚合物半导体材料,以其合适的能带结构和在可见光范围内的响应能力,展现出在光催化氧化还原反应中的广泛应用潜力,对治理环境污染和新能源技术开发具有显著意义.然而,含氮前驱体热聚合制备的体相g-C_(3)N_(4)存在可见光吸收范围窄、光生载流子快速复合和活性位点不足等局限性.为了克服这些限制,金属团簇与g-C_(3)N_(4)的结合被提出,并证明能显著增强其氧化还原性能.本文详细介绍了金属团簇的分类,并综述了通过构建异质结构、元素掺杂和缺陷工程等手段对g-C_(3)N_(4)进行改性的策略.针对各种改性策略,本文进行了详尽的分类和系统总结,涵盖了目前采用的制备方法及其对光催化剂性能提升的影响.此外,文章也指出了金属团簇改性g-C_(3)N_(4)在能源(如光催化产氢、CO_(2)还原)和环境(包括气体污染物去除、废水处理和有机污染物消除)领域应用中存在的挑战,并建议进一步研究改性策略及其制备方法,以期提高其在上述领域的应用效能,从而为未来研究提供方向.In recent years,industrialization and urbanization have led to global energy shortages and environmental pollution.There is an urgent need to explore new green technologies to address the energy and environmental crises.Semiconductor photocatalytic technology has been widely applied in various fields,such as carbon dioxide reduction to produce methane,water splitting to generate hydrogen or oxygen,and environmental purification,owing to its economic adaptability and mild reaction conditions.The rapid development of photocatalytic technology has become an effective means of solving energy and environmental issues,with the development of efficient photocatalysts at the core.Semiconductor graphitic carbon nitride(g-C_(3)N_(4))is an organic polymer semiconductor composed of sp2-hybridized carbon and nitrogen atoms interconnected by covalentσbonds andπbonds.It forms a network structure consisting of infinite extension of triazine or tri-s-triazine ring units.g-C_(3)N_(4)functions as a non-metallic and attractive photocatalytic material owing to its visible-light response,earth abundance,chemical-thermal stability and high yield.Therefore,g-C_(3)N_(4)is a suitable environmentally friendly photocatalysts.However,the C-N formingπ-conjugated planes along with relatively small electron mean free path(~10 nm)can result in the rapid recombination of photogenerated electron and hole pairs,which behaves with limited photocatalytic performance.Theoretically,g-C_(3)N_(4)shares the interlayer bonding form of van der Waals forces with graphene.Bulk g-C_(3)N_(4)samples prepared by the thermal polymerization of nitrogen-containing precursors,however,always exhibit limitations such as a narrow visible light absorption range and a deficiency of active sites.Therefore,we aim to tune the internal electron arrangement,change the surface microstructures,and create new and similar electron excitation orbital directions to improve the photocatalytic performance of g-C_(3)N_(4).Metal cluster modification exhibits high catalytic activity a

关 键 词：g-C_(3)N_(4) 金属团簇 光催化材料 改性策略 

分 类 号：O643.36[理学—物理化学] O644.1[理学—化学]