Significant Effect of Crystallization of Polymeric Carbon Nitride on Photoconductivity and Photocatalytic Activity for Visible-Light CO_(2)Reduction  

作　　者：Toshiya Tanaka Chao Zhang Ryuichi Nakada Jo Onodera Fumitaka Ishiwari Megumi Okazaki Akinori Saeki Osamu Ishitani Guigang Zhang Kazuhiko Maeda 

机构地区：[1]Department of Chemistry,School of Science,Institute of Science Tokyo,Meguro-ku,Tokyo 152-8550 [2]State Key Laboratory of Photocatalysis on Energy and Environment,College of Chemistry,Fuzhou University,Fuzhou 350002 [3]Department of Applied Chemistry,Graduate School of Engineering,Osaka University,Osaka 565-0871 [4]Innovative Catalysis Science Division,Institute for Open and Transdisciplinary Research Initiatives(ICS-OTRI),Osaka University,Osaka 565-0871 [5]PRESTO,Japan Science and Technology Agency(JST),Kawaguchi,Saitama 332-0012 [6]Department of Chemistry,Graduate School of Advanced Science and Engineering,Hiroshima University,Higashi-Hiroshima,Hiroshima 739-8526 [7]Research Center for Autonomous Systems Materialogy(ASMat),Institute of Science Tokyo,Yokohama,Kanagawa 226-8501

出　　处：《CCS Chemistry》2024年第12期2940-2949,共10页中国化学会会刊(英文)

基　　金：the National Natural Science Foundation of China(grant no.22311540011);the Japan Society for the Promotion of Science Grants-in-Aid for Scientific Research(JSPS KAKENHI;grant nos.JPJSBP120237406,JP22H05148,JP23H04626,and JP20H05836);supported by the Japan Science and Technology Support for Pioneering Research Initiated by the Next Generation(JST SPRING;grant no.JPMJSP2106).

摘　　要：The effect of crystallization of polymeric carbon nitride(PCN)on the photocatalytic CO_(2)reduction activity of a three-component hybrid comprising a Ru(II)binuclear complex(RuRu),Ag nanoparticles,and PCN,was investigated.Crystallized carbon nitride(CCN)obtained by heat treatment of PCN in a eutectic LiCl-KCl mixture was a much better hybrid photocatalyst component than the poorly crystallized PCN.The photocatalytic activity of CCN was dependent on the temperature of the LiCl-KCl treatment:Increasing the treatment temperature improved the photocatalytic activity as much as five-fold;however,treatment at elevated temperatures(>798 K)had a detrimental effect.Also,a substantial PCN crystallization effect was promoted by the construction of another hybrid photocatalyst from a mononuclear Ru(II)complex catalyst.Time-resolved microwave photoconductivity measurements revealed a good correlation between the photocatalytic activity and the photoconductivity-charge carrier lifetime product in the CCN samples heated at milder temperatures(≤798 K).For CCN specimens heated at higher temperatures,appreciable electron accumulation was observed during the photocatalytic reaction,indicating that the accumulated electrons could not participate in the CO_(2)reduction reaction.Thus,the crystallization of PCN at milder temperatures improved the mobility and lifetime of photogenerated charge carriers,thereby contributing to enhanced photocatalytic activity toward CO_(2)reduction.

关 键 词：artificial photosynthesis hydrogen carrier organic semiconductor solar fuels Z-scheme 

分 类 号：O62[理学—有机化学]