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
The random mobility of charge carriers is a main factor causing the low photocatalytic efficiency of gCN.Thus,the controllable migration of charge carriers is a rational strategy to suppress the charge recombination a...The random mobility of charge carriers is a main factor causing the low photocatalytic efficiency of gCN.Thus,the controllable migration of charge carriers is a rational strategy to suppress the charge recombination and facilitate charge separation.Herein,an ethylenediamine modified g-C_(3)N_(4)displays improved photocatalytic activity.The excellent charge separation efficiency is confirmed to be a key factor for the enhancement.The TEM observation after photo-depositing Pt nanoparticles and DFT calculations verify the accumulation of electrons on some areas of g-C_(3)N_(4)surface.The increased-NH_(2)groups significantly tune the electronic structure of g-C_(3)N_(4)after the modification.The generation of midgap states also affects the charge separation.Our reports provide a simple method to manage the migration of charge carriers and enable electrons directional transfer,which suppresses the recombination and improves the photocatalytic activity.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 Shenzhen Key Laboratory of Solid State Batteries(ZDSYS20180208184346531)Guangdong Provincial Key Laboratory of Energy Materials for Electric Power(2018B030322001)+3 种基金Guangdong Provincial Key Laboratory of Catalysis(2020B121201002)Shenzhen Clean Energy Research Institute(CERI-KY-2019-003)the National Natural Science Foundation of China(2017M611446)supported by the Core Research Facilities at SUSTech that receives support from a Presidential fund and the Development and Reform Commission of Shenzhen Municipality。
文摘The random mobility of charge carriers is a main factor causing the low photocatalytic efficiency of gCN.Thus,the controllable migration of charge carriers is a rational strategy to suppress the charge recombination and facilitate charge separation.Herein,an ethylenediamine modified g-C_(3)N_(4)displays improved photocatalytic activity.The excellent charge separation efficiency is confirmed to be a key factor for the enhancement.The TEM observation after photo-depositing Pt nanoparticles and DFT calculations verify the accumulation of electrons on some areas of g-C_(3)N_(4)surface.The increased-NH_(2)groups significantly tune the electronic structure of g-C_(3)N_(4)after the modification.The generation of midgap states also affects the charge separation.Our reports provide a simple method to manage the migration of charge carriers and enable electrons directional transfer,which suppresses the recombination and improves the photocatalytic activity.