Nanoparticle photosensitizers possess technical advantages for photocatalytic reactions due to enhanced light harvesting and efficient charge transport.Here we report synthesis of semiconductor nanoparticles through c...Nanoparticle photosensitizers possess technical advantages for photocatalytic reactions due to enhanced light harvesting and efficient charge transport.Here we report synthesis of semiconductor nanoparticles through covalent coupling and assembly of metalloporphyrin with condensed carbon nitride.The resultant nanoparticles consist of light harvesting component from the condensed carbon nitride and photocatalytic sites from the metalloporphyrins.This synergetic particle system effectively initiates efficient charge separation and transport and exhibits excellent photocatalytic activity for CO2 reduction.The CO production rate can reach up to 57μmol/(g·h)with a selectivity of 79%over competing H2 evolution.Controlled experiments demonstrate that the combination of light harvesting with photocatalytic activity via covalent assembly is crucial for the high photocatalytic activity.Due to effective charge separation and transfer,the resultant nanoparticle photocatalysts show exceptional photo stability against photo-corrosion under light irradiation,enabling for long-term utilization.This research opens a new way for the development of stable,effective nanoparticle photocatalysts using naturally abundant porphyrin pigments.展开更多
In order to broaden the absorption range of graphitic carbon nitride,one of the common methods is to couple the well-known photosensitizer porphyrin with graphitic carbon nitride through van der Waals weak in teractio...In order to broaden the absorption range of graphitic carbon nitride,one of the common methods is to couple the well-known photosensitizer porphyrin with graphitic carbon nitride through van der Waals weak in teractions.To date,to combine porphyrin with graphitic carbon nitridethrough covalent in teractions has not been settled.In this work,through rational molecular design,we successfully in corporated porphyrininto the matrixes of graphitic carbon nitride by covale nt bonding via on expot thermal copolymerization.The resulta nt material not only can wide nthe absorption range but also possess the enlarged specific surface area and construction intramolecular heterojunctions which can contributeto improve electron-holes separation efficiency.The resultant photocatalyst exhibited enhanced H2 production rate(7.6 mmol·g^-1·h^-1)and withthe apparent quantum efficiency(AQE)of 13.3%at 450 nm.At the same time,this method opens a way to fabricate graphitic carb on nitridenano sheets via bottom-up strategy.展开更多
基金E B.acknowledges the support from the National Natural Science Foundation of China(Nos.21771055 and U1604139)Zhongyuan high level talents special support plan(No.204200510010)Scientific and Technological Innovation Team in University of Henan Province(No.20IRTSTHN001).
文摘Nanoparticle photosensitizers possess technical advantages for photocatalytic reactions due to enhanced light harvesting and efficient charge transport.Here we report synthesis of semiconductor nanoparticles through covalent coupling and assembly of metalloporphyrin with condensed carbon nitride.The resultant nanoparticles consist of light harvesting component from the condensed carbon nitride and photocatalytic sites from the metalloporphyrins.This synergetic particle system effectively initiates efficient charge separation and transport and exhibits excellent photocatalytic activity for CO2 reduction.The CO production rate can reach up to 57μmol/(g·h)with a selectivity of 79%over competing H2 evolution.Controlled experiments demonstrate that the combination of light harvesting with photocatalytic activity via covalent assembly is crucial for the high photocatalytic activity.Due to effective charge separation and transfer,the resultant nanoparticle photocatalysts show exceptional photo stability against photo-corrosion under light irradiation,enabling for long-term utilization.This research opens a new way for the development of stable,effective nanoparticle photocatalysts using naturally abundant porphyrin pigments.
文摘In order to broaden the absorption range of graphitic carbon nitride,one of the common methods is to couple the well-known photosensitizer porphyrin with graphitic carbon nitride through van der Waals weak in teractions.To date,to combine porphyrin with graphitic carbon nitridethrough covalent in teractions has not been settled.In this work,through rational molecular design,we successfully in corporated porphyrininto the matrixes of graphitic carbon nitride by covale nt bonding via on expot thermal copolymerization.The resulta nt material not only can wide nthe absorption range but also possess the enlarged specific surface area and construction intramolecular heterojunctions which can contributeto improve electron-holes separation efficiency.The resultant photocatalyst exhibited enhanced H2 production rate(7.6 mmol·g^-1·h^-1)and withthe apparent quantum efficiency(AQE)of 13.3%at 450 nm.At the same time,this method opens a way to fabricate graphitic carb on nitridenano sheets via bottom-up strategy.
