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 nitri...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.展开更多
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).
文摘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.
基金supported by the Project of the National Nature Science Foundation of China(20531060 , 20418001 , 20473102)the National Basic Research 973 Program of China (2005CB623602 and 2006CB806201)National Center for Nanoscience and Technology,China
