The high exciton binding energy and lack of a positive oxidation band potential restrict the photocatalytic CO_(2)reduction efficiency of lead-free Bi-based halide perovskites Cs_(3)Bi_(2)X_(9)(X=Br,I).In this study,a...The high exciton binding energy and lack of a positive oxidation band potential restrict the photocatalytic CO_(2)reduction efficiency of lead-free Bi-based halide perovskites Cs_(3)Bi_(2)X_(9)(X=Br,I).In this study,a sequential growth method is presented to prepare a visible-light-driven(λ>420 nm)Z-scheme heterojunction photocatalyst composed of BiVO_(4)nanocrystals decorated on a Cs_(3)Bi_(2)I_(9)nanosheet for photocatalytic CO_(2)reduction coupled with water oxidation.The Cs_(3)Bi_(2)I_(9)/BiVO_(4)Z-scheme heterojunction photocatalyst is stable in the gas-solid photocatalytic CO_(2)reduction system,demonstrating a high visible-light-driven photocatalytic CO_(2)-to-CO production rate of 17.5μmol/(g·h),which is approximately three times that of pristine Cs_(3)Bi_(2)I_(9).The high efficiency of the Cs_(3)Bi_(2)I_(9)/BiVO_(4)heterojunction was attributed to the improved charge separation in Cs_(3)Bi_(2)I_(9).Moreover,the Z-scheme charge-transfer pathway preserves the negative reduction potential of Cs_(3)Bi_(2)I_(9)and the positive oxidation potential of BiVO_()4.This study off ers solid evidence of constructing Z-scheme heterojunctions to improve the photocatalytic performance of lead-free halide perovskites and would inspire more ideas for developing leadfree halide perovskite photocatalysts.展开更多
Chitosan(CS),hydrated zinc acetate,and rectorite(REC) were used as raw materials to prepare CS-embedded zinc oxide(ZnO) nanoparticle by a chemical precipitation process.Hydrogen-bonded REC-loaded ZnO-CS nanoparticle w...Chitosan(CS),hydrated zinc acetate,and rectorite(REC) were used as raw materials to prepare CS-embedded zinc oxide(ZnO) nanoparticle by a chemical precipitation process.Hydrogen-bonded REC-loaded ZnO-CS nanoparticle was to form ZnO-CS/REC nanocomposite photocatalyst,its morphology and structure were analyzed by means of FTIR,XRD,TGA,SEM,and TEM.The effects of the catalyst dosage,methyl orange(MO) initial concentration and solution pH on photocatalytic performance were also discussed.The experimental results show that the ZnO-CS/REC nanocomposite has a particle size of 100 nm with good dispersion and uniformity.Under irradiation of visible light,0.6 g/L photocatalyst was used to degrade MO in solution for 90 min at pH 6,then the MO solution(10 mg/L) was decolored by more than 99%,indicating that the ZnO-CS/REC nanocomposite exhibited highly photocatalytic degradation activity.Therefore,the photodegradation kinetic mechanism of MO in aqueous solution is presumed.展开更多
In this work,γ-Al_2O_3 and hydrogen peroxide treated g-C_3N_4(O-g-C_3N_4) were combined through a novel in-situ hydrothermal method to form heterojunction structured photocatalysts.These photocatalysts were character...In this work,γ-Al_2O_3 and hydrogen peroxide treated g-C_3N_4(O-g-C_3N_4) were combined through a novel in-situ hydrothermal method to form heterojunction structured photocatalysts.These photocatalysts were characterized by X-ray diffraction(XRD),scanning electron microscopy(SEM),Fourier transform infrared spectroscopy(FT-IR),X-ray photoelectron spectroscopy(XPS),UV–vis diffuse reflectance spectroscopy and photoluminescence spectroscopy(PL).FT-IR results indicate that oxygen functional groups can be grafted on the surface of O-g-C_3N_4 by hydrogen peroxide treatment.The visible light photocatalytic hydrogen evolution rate was investigated in 10 vol% TEOA aqueous solution.The optimal Al_2O_3 mass content is set to be 20 wt% and the corresponding hydrogen evolution rate is 1288 μmol/h/g which is approximately 6,3 folds that of pristine g-C_3N_4 and O-g-C_3N_4 respectively and 1.6 folds that of mechanical mixed composite with the same Al_2O_3 mass content.The photocurrent density–time curves were carried out under visible light illumination for four on–off cycles.The electrochemical impedance spectroscopy(EIS) measurements verified the enhanced separation efficiency of electron–hole pairs.This work raised a new method to form the heterojunction structured photocatalysts and achieved a remarkable improvement of the photocatalytic activity in water splitting for hydrogen under visible light irradiation.展开更多
This paper conducts a research on modulation characteristics of blue light-emitting diodes (LEDs) used in a visible-light communication (VLC) system. Through analysis of the modulation characteristics of LEDs with dif...This paper conducts a research on modulation characteristics of blue light-emitting diodes (LEDs) used in a visible-light communication (VLC) system. Through analysis of the modulation characteristics of LEDs with different emitting sizes, we find that there is a similar linear relationship between LED’s 3dB bandwidth and the operation current density. This experiment also shows that high series resistance is one major issue that limits our LED's modulation speed. To further improve the LED bandwidth, the resistance can be reduced by optimizing device layout as well as reducing material bulk resistance. Clearly, this study provides an approach to increase the modulation bandwidth of GaN-based LEDs for VLC systems.展开更多
Flow cytometric (FCM) and microspectrophotometric (MSP) measurements of cell nuclear DNA content were made in 53 fresh gastric carcinoma specimens and in 30 gastric mucosal specimens with chronic gastritis. DNA aneupl...Flow cytometric (FCM) and microspectrophotometric (MSP) measurements of cell nuclear DNA content were made in 53 fresh gastric carcinoma specimens and in 30 gastric mucosal specimens with chronic gastritis. DNA aneuploidy was found in 32/53 (60%) of gastric carcinomas, and appeared more frequently in wellor moderately differentiated tubular adenocarcinomas (90%) than in undifferentiated and mucousa cell carcinomas (23.6%) (P【0.001). No aneuploidy was found in chronic gastritis samples, but their proliferative cell fractions were higher than in normal control gastric mucosa samples (P【0.01). A comparison was made between FCM and MSP analyses of DNA content in 29 cases of gastric carcinoma, a high correlation rate (r=0.90) was found. The advantages and limitations of both methods are discussed, they may be used in combination for more precise cytochemical analysis.展开更多
We demonstrate visible-light all-fiber vortex lasers by incorporating the home-made mode selective couplers (MSCs). The MSC at green or red wavebands is fabricated by specially designing and fusing a single-mode fiber...We demonstrate visible-light all-fiber vortex lasers by incorporating the home-made mode selective couplers (MSCs). The MSC at green or red wavebands is fabricated by specially designing and fusing a single-mode fiber (SMF) and a few-mode fiber (FMF). The MSCs inserted into visible fiber cavities act as power splitters and mode converters from the LP01 to LP11 mode at green and red wavelengths, respectively. The red-light all-fiber vortex laser is formed by a 10-cm Pr3+/Yb3+:ZBLAN fiber, a fiber Bragg grating, a fiber end-facet mirror and the MSC at 635 nm, which generates vortex beams with OAM±1 at 634.4 nm and an output power of 13 mW. The green-light all-fiber vortex laser consists of a 12-cm Ho3+:ZBLAN fiber, two fiber pigtail mirrors, and the MSC at 550 nm, which generates vortex beams with OAM±1 at 548.9 nm and an output power of 3 mW.展开更多
Integrating the advantages of Bi and Cr elements in the bandgap engineering of metal oxides, a visible-light-responsive photocatalyst Bi1.5Cr0.5WO6 is successfully constructed and initially applied in water decontamin...Integrating the advantages of Bi and Cr elements in the bandgap engineering of metal oxides, a visible-light-responsive photocatalyst Bi1.5Cr0.5WO6 is successfully constructed and initially applied in water decontamination. The combination of UV-vis diffuses reflectance and the Mott-Schottky curve from electrochemical testing can be used to determine the conduction band and valence band of Bi1.5Cr0.5WO6 to be about –1.26 and 1.42 V, respectively. The location of energy band structure indicates that the superoxide free radical can be produced in Bi1.5Cr0.5WO6 photocatalytic system without hydroxyl group. This speculation is also confirmed by ESR experiment and active radical species scavenging experiments. In addition, the best photocatalytic performance of Bi1.5Cr0.5WO6 obtained under 180 ℃ is attributed to the smallest impedance and the strongest electronic migration capability.展开更多
The rare earth ion Yb^3+ doped Bi2WO6 photocatalysts were synthesized by hydrothermal method.Moreover,XRD,XPS,FESEM,TEM,Ramam,N2 adsorption-desorption isotherm measurements and UV-vis diffusion reflectance spectra wer...The rare earth ion Yb^3+ doped Bi2WO6 photocatalysts were synthesized by hydrothermal method.Moreover,XRD,XPS,FESEM,TEM,Ramam,N2 adsorption-desorption isotherm measurements and UV-vis diffusion reflectance spectra were used to characterize the Yb^3+ doped Bi2WO6 photocatalysts.The morphology,specific surface area,and pore volume distribution were greatly affected after Yb3+ ions doping.Photocatalytic performance of Bi2WO6 was effectively enhanced after Yb3+ ions doping,6% Yb^3+ doped Bi2WO6 had the best photocatalytic performance,and 96.2% Rhodamine B was degradated after irradiated 30 min,which was 1.29 times that of the pristine one.The enhanced photocatalytic performance was due to the increased specific surface area,decreased energy band gap and inhibition of photoelectron-hole recombination after Yb3+ ions doping.展开更多
Photocatalysis is one of the most promising methods owing to its great potential to relieve environmental issue. To construct efficient photocatalyst with low energy consumption, mild catalytic conditions, and stable ...Photocatalysis is one of the most promising methods owing to its great potential to relieve environmental issue. To construct efficient photocatalyst with low energy consumption, mild catalytic conditions, and stable chemical properties are highly desired. In this work, a novel, highly active and environmental friendly mesoporous photocatalyst Bi4O5Br2/SBA-15 was synthesized by hydrothermal method, and its characteristics and visible-light catalytic activity were investigated. The synthesized photocatalyst consisted of Langmuir type IV hysteresis loops, which was confirmed to be a composite material with mesoporous structure. It exhibited a high visible-light absorption intensity and a low recombination rate of photo-generated electrons and holes. When the mass ratio of Bi/SiO2 was 30/100 during the synthesis, the obtained photocatalyst (Bi30/SBA-15) reflected the fastest Rhodamine B (RhB) removal rate and achieved 100% decolorization of RhB by both adsorption and degradation process. This high decolorization efficiency can also be maintained and realized by recycling the used composite in practice. The enhanced visible-light photocatalytic activity of novel Bi4O5Br2/SBA-15 photocatalyst can be ascribed to the existing active sites both inside and outside SBA-15 which enhanced the separation of photo-generated electrons and holes.展开更多
Two-dimensional(2D)carbon nitride sheets(CNs)with atomically thin structures are regarded as one of the most promising materials for solar energy conversion.However,due to their substantially enlarged bandgap caused b...Two-dimensional(2D)carbon nitride sheets(CNs)with atomically thin structures are regarded as one of the most promising materials for solar energy conversion.However,due to their substantially enlarged bandgap caused by the strong quantum size effect and their incomplete polymerisation with a large number of non-condensed surface amino groups,the practical applicability of CNs in photocatalysis is limited.In this study,CNs with broad visible-light absorption were synthesised using a 5-min fast thermal annealing.The removal of uncondensed amine groups reduces the bandgap of CNs from 3.06 eV to 2.60 eV,increasing their absorption of visible light.Interestingly,the CNs were distorted after annealing,which can differentiate the spatial positions of electrons and holes,enhancing the visible-light absorption efficiency.As a result,when exposed to visible light,the photocatalytic hydrogen production activity of atomically thin 2D CNs rose by 8.38 times.This research presents a dependable and speedy method for creating highly effective visible-light photocatalysts with narrowed bandgaps and improved visible-light absorption.展开更多
An additive-free and environmentally friendly strategy has been realized for the construction of S-substituted isothioureas through visible-light-induced multicomponent reaction starting fromα-diazoesters,aryl isothi...An additive-free and environmentally friendly strategy has been realized for the construction of S-substituted isothioureas through visible-light-induced multicomponent reaction starting fromα-diazoesters,aryl isothiocyanates,amines and cyclic ethers.This methodology features simple operation,mild reaction conditions,favorable functional group tolerance,easily available starting materials and high efficiency.展开更多
N-formylation of amines,a class of synthetically important reactions,is typically conducted using metal catalysts that are relatively expensive or not readily available and usually needs harsh conditions to increase t...N-formylation of amines,a class of synthetically important reactions,is typically conducted using metal catalysts that are relatively expensive or not readily available and usually needs harsh conditions to increase the reaction efficiency.Here,an efficient continuous microflow strategy was developed for the gas-liquid visible-light photocatalytic N-formylation of piperidine,which achieved a reaction yield of 82.97%and a selectivity of>99%at 12 min using cheap organic dye photocatalyst under mild reaction conditions.The influence of essential parameters,including light intensity,temperature and equivalents of the gas,additive and photocatalyst,on the reaction yield was systematically studied.Furthermore,kinetic investigations were conducted,exhibiting the dependence of reaction rate and equilibrium yield of N-formylpiperidine on light intensity,temperature and photocatalyst equivalent.The microflow photocatalytic approach established in this work,which realized a markedly higher space-time yield than the conventional batch method(37.9 vs.0.212 mmol h-1 L-1),paves the way for the continuous,green and efficient synthesis of N-formamides.展开更多
基金support from the National Key R&D Plan Project(No.2022YFA1505000)Prospective Basic Research Projects of CNPC(Nos.2021DQ03(2022Z-29)+4 种基金2022DJ5406,2022DJ5407,2022DJ5408,2022DJ4507,and TGRI-2021-1)the Natural Science Foundation of Shaanxi Province(No.2022JQ-078)the Natural Science Foundation of China(No.52302308)the Outstanding Youth Science Foundation Project of the National Natural Science Foundation of China(Overseas)(No.GYKP033)the Qinchuangyuan Cited High-Level Innovative and Entrepreneurial Talents Project(No.QCYRCXM-2022-143).
文摘The high exciton binding energy and lack of a positive oxidation band potential restrict the photocatalytic CO_(2)reduction efficiency of lead-free Bi-based halide perovskites Cs_(3)Bi_(2)X_(9)(X=Br,I).In this study,a sequential growth method is presented to prepare a visible-light-driven(λ>420 nm)Z-scheme heterojunction photocatalyst composed of BiVO_(4)nanocrystals decorated on a Cs_(3)Bi_(2)I_(9)nanosheet for photocatalytic CO_(2)reduction coupled with water oxidation.The Cs_(3)Bi_(2)I_(9)/BiVO_(4)Z-scheme heterojunction photocatalyst is stable in the gas-solid photocatalytic CO_(2)reduction system,demonstrating a high visible-light-driven photocatalytic CO_(2)-to-CO production rate of 17.5μmol/(g·h),which is approximately three times that of pristine Cs_(3)Bi_(2)I_(9).The high efficiency of the Cs_(3)Bi_(2)I_(9)/BiVO_(4)heterojunction was attributed to the improved charge separation in Cs_(3)Bi_(2)I_(9).Moreover,the Z-scheme charge-transfer pathway preserves the negative reduction potential of Cs_(3)Bi_(2)I_(9)and the positive oxidation potential of BiVO_()4.This study off ers solid evidence of constructing Z-scheme heterojunctions to improve the photocatalytic performance of lead-free halide perovskites and would inspire more ideas for developing leadfree halide perovskite photocatalysts.
基金the National Key Research and Development Project(2019YFC1908204)the Fund of Key Laboratory of Measurement and Control System for Offshore Environment(Fuqing Branch of Fujian Normal University)(No.SI-KF1604)+2 种基金the Key Project of Science and Technology Department of Fujian Province(No.2018H0013)the Key Natural Fund Project of Universities in Fujian Province(No.JZ160490)the Fuqing Branch of Fujian Normal University Cultivation Project(Nos.KY2017NS06,KY201609)。
文摘Chitosan(CS),hydrated zinc acetate,and rectorite(REC) were used as raw materials to prepare CS-embedded zinc oxide(ZnO) nanoparticle by a chemical precipitation process.Hydrogen-bonded REC-loaded ZnO-CS nanoparticle was to form ZnO-CS/REC nanocomposite photocatalyst,its morphology and structure were analyzed by means of FTIR,XRD,TGA,SEM,and TEM.The effects of the catalyst dosage,methyl orange(MO) initial concentration and solution pH on photocatalytic performance were also discussed.The experimental results show that the ZnO-CS/REC nanocomposite has a particle size of 100 nm with good dispersion and uniformity.Under irradiation of visible light,0.6 g/L photocatalyst was used to degrade MO in solution for 90 min at pH 6,then the MO solution(10 mg/L) was decolored by more than 99%,indicating that the ZnO-CS/REC nanocomposite exhibited highly photocatalytic degradation activity.Therefore,the photodegradation kinetic mechanism of MO in aqueous solution is presumed.
基金supported by the National Scientific Foundation of China(NSFC,Project no.21306119)the Provincial Natural Science Foundation of Sichuan(2013FZ0034 and 2013JY0150)the Outstanding Young Scientist Foundation of Sichuan University(2013SCU04A23)
文摘In this work,γ-Al_2O_3 and hydrogen peroxide treated g-C_3N_4(O-g-C_3N_4) were combined through a novel in-situ hydrothermal method to form heterojunction structured photocatalysts.These photocatalysts were characterized by X-ray diffraction(XRD),scanning electron microscopy(SEM),Fourier transform infrared spectroscopy(FT-IR),X-ray photoelectron spectroscopy(XPS),UV–vis diffuse reflectance spectroscopy and photoluminescence spectroscopy(PL).FT-IR results indicate that oxygen functional groups can be grafted on the surface of O-g-C_3N_4 by hydrogen peroxide treatment.The visible light photocatalytic hydrogen evolution rate was investigated in 10 vol% TEOA aqueous solution.The optimal Al_2O_3 mass content is set to be 20 wt% and the corresponding hydrogen evolution rate is 1288 μmol/h/g which is approximately 6,3 folds that of pristine g-C_3N_4 and O-g-C_3N_4 respectively and 1.6 folds that of mechanical mixed composite with the same Al_2O_3 mass content.The photocurrent density–time curves were carried out under visible light illumination for four on–off cycles.The electrochemical impedance spectroscopy(EIS) measurements verified the enhanced separation efficiency of electron–hole pairs.This work raised a new method to form the heterojunction structured photocatalysts and achieved a remarkable improvement of the photocatalytic activity in water splitting for hydrogen under visible light irradiation.
文摘This paper conducts a research on modulation characteristics of blue light-emitting diodes (LEDs) used in a visible-light communication (VLC) system. Through analysis of the modulation characteristics of LEDs with different emitting sizes, we find that there is a similar linear relationship between LED’s 3dB bandwidth and the operation current density. This experiment also shows that high series resistance is one major issue that limits our LED's modulation speed. To further improve the LED bandwidth, the resistance can be reduced by optimizing device layout as well as reducing material bulk resistance. Clearly, this study provides an approach to increase the modulation bandwidth of GaN-based LEDs for VLC systems.
文摘Flow cytometric (FCM) and microspectrophotometric (MSP) measurements of cell nuclear DNA content were made in 53 fresh gastric carcinoma specimens and in 30 gastric mucosal specimens with chronic gastritis. DNA aneuploidy was found in 32/53 (60%) of gastric carcinomas, and appeared more frequently in wellor moderately differentiated tubular adenocarcinomas (90%) than in undifferentiated and mucousa cell carcinomas (23.6%) (P【0.001). No aneuploidy was found in chronic gastritis samples, but their proliferative cell fractions were higher than in normal control gastric mucosa samples (P【0.01). A comparison was made between FCM and MSP analyses of DNA content in 29 cases of gastric carcinoma, a high correlation rate (r=0.90) was found. The advantages and limitations of both methods are discussed, they may be used in combination for more precise cytochemical analysis.
基金Project supported by the National Natural Science Foundation of China(Grant Nos.91750115 and 91750108)the Equipment Pre-research Project of Equipment Development Department of Central Military Commission,China(Grant No.61404140112)the Science and Technology Planning Project of Xiamen City,China(Grant No.3502Z20183003).
文摘We demonstrate visible-light all-fiber vortex lasers by incorporating the home-made mode selective couplers (MSCs). The MSC at green or red wavebands is fabricated by specially designing and fusing a single-mode fiber (SMF) and a few-mode fiber (FMF). The MSCs inserted into visible fiber cavities act as power splitters and mode converters from the LP01 to LP11 mode at green and red wavelengths, respectively. The red-light all-fiber vortex laser is formed by a 10-cm Pr3+/Yb3+:ZBLAN fiber, a fiber Bragg grating, a fiber end-facet mirror and the MSC at 635 nm, which generates vortex beams with OAM±1 at 634.4 nm and an output power of 13 mW. The green-light all-fiber vortex laser consists of a 12-cm Ho3+:ZBLAN fiber, two fiber pigtail mirrors, and the MSC at 550 nm, which generates vortex beams with OAM±1 at 548.9 nm and an output power of 3 mW.
基金financially supported by the Natural Science Foundation of Fujian province(2016J05042,2015J01057,2018J01439)Open Fund of State Key Laboratory of Photocatalysis on Energy and Environment(SKLPEE-KF201505)+3 种基金Scientific Project of Putian Science and Technology Bureau(2016S1001)Science and Technology Project of Fujian Provincial Department of Education(JA15444)the Projects of Putian University(2015065,2015081)Program for New Century Excellent Talents in Fujian Province University
文摘Integrating the advantages of Bi and Cr elements in the bandgap engineering of metal oxides, a visible-light-responsive photocatalyst Bi1.5Cr0.5WO6 is successfully constructed and initially applied in water decontamination. The combination of UV-vis diffuses reflectance and the Mott-Schottky curve from electrochemical testing can be used to determine the conduction band and valence band of Bi1.5Cr0.5WO6 to be about –1.26 and 1.42 V, respectively. The location of energy band structure indicates that the superoxide free radical can be produced in Bi1.5Cr0.5WO6 photocatalytic system without hydroxyl group. This speculation is also confirmed by ESR experiment and active radical species scavenging experiments. In addition, the best photocatalytic performance of Bi1.5Cr0.5WO6 obtained under 180 ℃ is attributed to the smallest impedance and the strongest electronic migration capability.
基金the National Natural Science Foundation of China(No.51662005)。
文摘The rare earth ion Yb^3+ doped Bi2WO6 photocatalysts were synthesized by hydrothermal method.Moreover,XRD,XPS,FESEM,TEM,Ramam,N2 adsorption-desorption isotherm measurements and UV-vis diffusion reflectance spectra were used to characterize the Yb^3+ doped Bi2WO6 photocatalysts.The morphology,specific surface area,and pore volume distribution were greatly affected after Yb3+ ions doping.Photocatalytic performance of Bi2WO6 was effectively enhanced after Yb3+ ions doping,6% Yb^3+ doped Bi2WO6 had the best photocatalytic performance,and 96.2% Rhodamine B was degradated after irradiated 30 min,which was 1.29 times that of the pristine one.The enhanced photocatalytic performance was due to the increased specific surface area,decreased energy band gap and inhibition of photoelectron-hole recombination after Yb3+ ions doping.
文摘Photocatalysis is one of the most promising methods owing to its great potential to relieve environmental issue. To construct efficient photocatalyst with low energy consumption, mild catalytic conditions, and stable chemical properties are highly desired. In this work, a novel, highly active and environmental friendly mesoporous photocatalyst Bi4O5Br2/SBA-15 was synthesized by hydrothermal method, and its characteristics and visible-light catalytic activity were investigated. The synthesized photocatalyst consisted of Langmuir type IV hysteresis loops, which was confirmed to be a composite material with mesoporous structure. It exhibited a high visible-light absorption intensity and a low recombination rate of photo-generated electrons and holes. When the mass ratio of Bi/SiO2 was 30/100 during the synthesis, the obtained photocatalyst (Bi30/SBA-15) reflected the fastest Rhodamine B (RhB) removal rate and achieved 100% decolorization of RhB by both adsorption and degradation process. This high decolorization efficiency can also be maintained and realized by recycling the used composite in practice. The enhanced visible-light photocatalytic activity of novel Bi4O5Br2/SBA-15 photocatalyst can be ascribed to the existing active sites both inside and outside SBA-15 which enhanced the separation of photo-generated electrons and holes.
基金supported by the National Natural Science Foundation of China(Nos.12104352 and 12204294)Fundamental Research Funds for the Central Universities(Nos.XJS_(2)12208 and 2020BJ-56)+1 种基金Foundation of State Key Laboratory of High-efficiency Utilization of Coal and Green Chemical Engineering(No.2022-K67)the Natural Science Foundation of Shaanxi Province(Nos.2019JCW-17 and 2020JCW-15).
文摘Two-dimensional(2D)carbon nitride sheets(CNs)with atomically thin structures are regarded as one of the most promising materials for solar energy conversion.However,due to their substantially enlarged bandgap caused by the strong quantum size effect and their incomplete polymerisation with a large number of non-condensed surface amino groups,the practical applicability of CNs in photocatalysis is limited.In this study,CNs with broad visible-light absorption were synthesised using a 5-min fast thermal annealing.The removal of uncondensed amine groups reduces the bandgap of CNs from 3.06 eV to 2.60 eV,increasing their absorption of visible light.Interestingly,the CNs were distorted after annealing,which can differentiate the spatial positions of electrons and holes,enhancing the visible-light absorption efficiency.As a result,when exposed to visible light,the photocatalytic hydrogen production activity of atomically thin 2D CNs rose by 8.38 times.This research presents a dependable and speedy method for creating highly effective visible-light photocatalysts with narrowed bandgaps and improved visible-light absorption.
基金financially supported by Natural Science Foundation of Shandong Province(No.ZR2021MB065)the major innovation fund of Shandong Province(No.2021ZDSYS_(2)3)the National Natural Science Foundation of China(Nos.21976105,22101237).
文摘An additive-free and environmentally friendly strategy has been realized for the construction of S-substituted isothioureas through visible-light-induced multicomponent reaction starting fromα-diazoesters,aryl isothiocyanates,amines and cyclic ethers.This methodology features simple operation,mild reaction conditions,favorable functional group tolerance,easily available starting materials and high efficiency.
基金the financial support from the National Natural Science Foundation of China(No.21808059)the Fundamental Research Funds for the Central Universities(No.JKA01221712).
文摘N-formylation of amines,a class of synthetically important reactions,is typically conducted using metal catalysts that are relatively expensive or not readily available and usually needs harsh conditions to increase the reaction efficiency.Here,an efficient continuous microflow strategy was developed for the gas-liquid visible-light photocatalytic N-formylation of piperidine,which achieved a reaction yield of 82.97%and a selectivity of>99%at 12 min using cheap organic dye photocatalyst under mild reaction conditions.The influence of essential parameters,including light intensity,temperature and equivalents of the gas,additive and photocatalyst,on the reaction yield was systematically studied.Furthermore,kinetic investigations were conducted,exhibiting the dependence of reaction rate and equilibrium yield of N-formylpiperidine on light intensity,temperature and photocatalyst equivalent.The microflow photocatalytic approach established in this work,which realized a markedly higher space-time yield than the conventional batch method(37.9 vs.0.212 mmol h-1 L-1),paves the way for the continuous,green and efficient synthesis of N-formamides.