A facile method to introduce a donor-acceptor system into polymeric carbon nitride for efficient photocatalytic overall water splitting  

作　　者：Yabin Jiang Chi Cao Yueyang Tan Qianwen Chen Lei Zeng Wensheng Yang Zongzhao Sun Limin Huang 

机构地区：[1]School of Materials,Sun Yat-Sen University,Shenzhen 518107,China [2]Department of Chemistry,Southern University of Science and Technology,Shenzhen 518055,China [3]Engineering Research Center for Nanomaterials,Henan University,Kaifeng 475004,China [4]Institute of Molecular Plus,Tianjin University,Tianjin 300072,China [5]State Key Laboratory of Inorganic Synthesis and Preparative Chemistry,College of Chemistry,Jilin University,Changchun 130012,China

出　　处：《Journal of Materials Science & Technology》2023年第10期32-41,共10页材料科学技术（英文版）

基　　金：supported by the National Natural Science Foundation of China(Nos.21703097 and 21972172);South-ern University of Science and Technology(SUSTech)start fund through the Shenzhen Peacock Talent program,the Shenzhen Ba-sic Research Fund project(No.JCYJ20150507170334573);the Guangdong Innovative and Entrepreneurial Research Team Program(No.2016ZT06N532).

摘　　要：It is a prospective strategy to produce sustainable energy by photocatalytic overall water splitting(POWS).This work aims to develop a simple method for integrating a donor-acceptor system into polymeric car-bon nitride(PCN)structure,which could accelerate the charge separation significantly.In the as-prepared photocatalyst(COCNT),carbon and oxygen were successfully incorporated into the framework of PCN,and the chemical environment of C and O was well probed by X-ray absorption near-edge structure(XANES)and X-ray photoelectron spectroscopy(XPS).It showed that the C-containing and O-containing segments of COCNT played the role of a donor,while the heptazine part played the role of an acceptor.In addition,Density-functional-theory(DFT)calculations confirmed the spatial split of the highest occupied molec-ular orbital(HOMO)and lowest unoccupied molecular orbital(LUMO)for promoting charge separation.Impressively,COCNT could efficiently split pure water to generate hydrogen and oxygen.And,the photo-catalytic hydrogen evolution rate over COCNT(1550.9μmol g^(-1)h^(-1))is about 17-fold higher than that of PCN.Finally,we proposed a possible photocatalytic mechanism to explain the above results.

关 键 词：Polymeric carbon nitride Donor-accept system Tubular structure PHOTOCATALYSIS Overall water splitting 

分 类 号：O643.36[理学—物理化学] O644.1[理学—化学]