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
Intramolecular charge transfer(ICT)derived from a donor-acceptor system has been applied for years to enhance the charge mobility in the field of organic photovoltaics and chemical sensing.Similar strategies have grad...Intramolecular charge transfer(ICT)derived from a donor-acceptor system has been applied for years to enhance the charge mobility in the field of organic photovoltaics and chemical sensing.Similar strategies have gradually been developed in polymeric graphitic carbon nitride(GCN)photocatalytic systems for promoting the light absorption and charge separation.However,there are no reviews focusing on the effects of ICT after the modification of GCN so far.Herein,we summarize some typical literature on GCN engineering to expound profoundly the roles of ICT in electronic properties regulation in terms of in-situ formation and molecular coupling.At last,some important perspectives are also proposed.This review will deepen understanding of the traditional theory for a new recognition among such many methods to improve the performance of GCN.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This work was financially supported by Southern University of Science and Technology(SUSTech)start fund through Shenzhen Peacock Talent program,Guangdong Provincial Key Laboratory of Energy Materials for Electric Power(2018B030322001)Guangdong Provincial Key Laboratory of Catalysis(2020B121201002)+1 种基金Shenzhen Clean Energy Research Institute(CERI-KY-2019-003)Shenzhen Key Laboratory of Solid State Batteries(ZDSYS20180208184346531).
文摘Intramolecular charge transfer(ICT)derived from a donor-acceptor system has been applied for years to enhance the charge mobility in the field of organic photovoltaics and chemical sensing.Similar strategies have gradually been developed in polymeric graphitic carbon nitride(GCN)photocatalytic systems for promoting the light absorption and charge separation.However,there are no reviews focusing on the effects of ICT after the modification of GCN so far.Herein,we summarize some typical literature on GCN engineering to expound profoundly the roles of ICT in electronic properties regulation in terms of in-situ formation and molecular coupling.At last,some important perspectives are also proposed.This review will deepen understanding of the traditional theory for a new recognition among such many methods to improve the performance of GCN.
