Exclusive responsiveness to ultraviolet light (~3.2 eV) and high photogenerated charge recombination rate are the two primary drawbacks of pure TiO_(2). We combined N-doped graphene quantum dots (N-GQDs), morphology r...Exclusive responsiveness to ultraviolet light (~3.2 eV) and high photogenerated charge recombination rate are the two primary drawbacks of pure TiO_(2). We combined N-doped graphene quantum dots (N-GQDs), morphology regulation, and heterojunction construction strategies to synthesize N-GQD/N-doped TiO_(2)/P-doped porous hollow g-C_(3)N_(4) nanotube (PCN) composite photocatalysts (denoted as G-TPCN). The optimal sample (G-TPCN doped with 0.1wt% N-GQD, denoted as 0.1% G-TPCN) exhibits significantly enhanced photoabsorption, which is attributed to the change in bandgap caused by elemental doping (P and N), the improved light-harvesting resulting from the tube structure, and the upconversion effect of N-GQDs. In addition, the internal charge separation and transfer capability of0.1% G-TPCN are dramatically boosted, and its carrier concentration is 3.7, 2.3, and 1.9 times that of N-TiO_(2), PCN, and N-TiO_(2)/PCN(TPCN-1), respectively. This phenomenon is attributed to the formation of Z-scheme heterojunction between N-TiO_(2) and PCNs, the excellent electron conduction ability of N-GQDs, and the short transfer distance caused by the porous nanotube structure. Compared with those of N-TiO_(2), PCNs, and TPCN-1, the H2 production activity of 0.1%G-TPCN under visible light is enhanced by 12.4, 2.3, and 1.4times, respectively, and its ciprofloxacin (CIP) degradation rate is increased by 7.9, 5.7, and 2.9 times, respectively. The optimized performance benefits from excellent photoresponsiveness and improved carrier separation and migration efficiencies. Finally, the photocatalytic mechanism of 0.1% G-TPCN and five possible degradation pathways of CIP are proposed. This study clarifies the mechanism of multiple modification strategies to synergistically improve the photocatalytic performance of 0.1% G-TPCN and provides a potential strategy for rationally designing novel photocatalysts for environmental remediation and solar energy conversion.展开更多
Visible-light-driven photocatalysis is a promising technology for the treatment of dye wastewater.In this work,a novel photocatalyst of K-doped g-C_(3)N_(4) loaded on magnetic attapulgite(ATP)(Kω-g-C_(3)N_(4)@ATP-Fe_...Visible-light-driven photocatalysis is a promising technology for the treatment of dye wastewater.In this work,a novel photocatalyst of K-doped g-C_(3)N_(4) loaded on magnetic attapulgite(ATP)(Kω-g-C_(3)N_(4)@ATP-Fe_(3)O_(4))with excellent visible light photocatalytic properties and stability were successfully prepared and characterized.The removal efficiency of Kω-g-C_(3)N_(4)@ATP-Fe_(3)O_(4) for malachite green(MG)was studied,and the degradation mechanism was analyzed and proposed.It was found that the K_(5)-g-C_(3)N_(4)@ATP-Fe_(3)O_(4) photocatalyst possessed excellent degradation efficiency of over 98.0%for the MG dye wastewater under optimal conditions.Moreover,the K_(5)-g-C_(3)N_(4)@ATP-Fe_(3)O_(4) materials possessed good recyclability with a removal rate over 82%after 4 cycles.Under visible light condition,the K_(5)-g-C_(3)N_(4)@ATP-Fe_(3)O_(4) photocatalyst produce radicals of·OH and O_(2)^(-)to degrade the MG dyes,which was supported by electron paramagnetic resonance(EPR)and radical trapping experiments.In addition,the LC-MS analysis interpreted the degradation pathways and intermediates of MG in the solution.The findings in this work indicate that the prepared photocatalytic material has excellent degradation efficiency for MG and can be applied in dye wastewater treatment.展开更多
Photocatalysis driven by abundant yet intermittent solar energy has considerable potential in renewable energy generation and environmental remediation.The outstanding electronic structure and physicochemical properti...Photocatalysis driven by abundant yet intermittent solar energy has considerable potential in renewable energy generation and environmental remediation.The outstanding electronic structure and physicochemical properties of graphitic carbon nitride(g-C_(3)N_(4)),together with unique metal-free characteristic,make them ideal candidates for advanced photocatalysts construction.This review summarizes the up-to-date advances on g-C_(3)N_(4)based photocatalysts from ingenious-design strategies and diversified photocatalytic applications.Notably,the advantages,fabrication methods and limitations of each design strategy are systemically analyzed.In order to deeply comprehend the inner connection of theory–structure–performance upon g-C_(3)N_(4)based photocatalysts,structure/composition designs,corresponding photocatalytic activities and reaction mechanisms are jointly discussed,associated with introducing their photocatalytic applications toward water splitting,carbon dioxide/nitrogen reduction and pollutants degradation,etc.Finally,the current challenges and future perspectives for g-C_(3)N_(4)based materials for photocatalysis are briefly proposed.These design strategies and limitations are also instructive for constructing g-C_(3)N_(4) based materials in other energy and environment-related applications.展开更多
In this research study, we have synthesized the bio-capped ZnO/g-C_(3)N_(4) nanocomposites by employing lemon juice(Citrus limon) as a stabilizer and mediator. Fruitfully, lemon juice which contains various acidic fun...In this research study, we have synthesized the bio-capped ZnO/g-C_(3)N_(4) nanocomposites by employing lemon juice(Citrus limon) as a stabilizer and mediator. Fruitfully, lemon juice which contains various acidic functional groups and citric acid has the capability to block the surface of g-C_(3)N_(4) from chemical reactivity and activated the surface of g-C_(3)N_(4) for various reactions. Consequently, the agglomeration behavior and controlled shape of g-C_(3)N_(4) has also been achieved. Our experimental results i.e. XRD,TEM, HRTEM, PL, FS, XPS, and PEC have confirmed that the lemon juice mediated and green g-C_(3)N_(4)(L-CN) have good performances and remarkable visible light photocatalytic activities as compared to the chemically synthesized g-C_(3)N_(4)(CN). Furthermore, the small surface area and low charge separation of g-C_(3)N_(4) is upgraded by coupling with Zn O nanoparticles. It is proved that the coupling of Zn O worked as a facilitator and photoelectron modulator to enhance the charge separation of g-C_(3)N_(4). Compared to pristine lemon-mediated green g-C_(3)N_(4)(L-CN), the most active sample 5Zn O/L-CN showed ~ 5-fold improvement in activities for ciprofloxacin(CIP) and methylene blue(MB) degradation. More specifically,the mineralization process and degradation pathways, and the mineralization process of ciprofloxacin(CIP) and methylene blue(MB) are suggested. Finally, our present novel research work will provide new access to synthesize the eco-friendly and bio-caped green g-C_(3)N_(4)nanomaterials and their employment for pollutants degradation and environmental purification.展开更多
Novel graphitic carbon nitride(g-C_(3)N_(4))nanosheet/Bi_(5)O_(7)Br/NH_(2)-MIL-88B(Fe)photocatalysts(denoted as GCN-NSh/Bi_(5)O_(7)Br/FeMOF,in which MOF is metal–organic framework)with double S-scheme heterojunctions...Novel graphitic carbon nitride(g-C_(3)N_(4))nanosheet/Bi_(5)O_(7)Br/NH_(2)-MIL-88B(Fe)photocatalysts(denoted as GCN-NSh/Bi_(5)O_(7)Br/FeMOF,in which MOF is metal–organic framework)with double S-scheme heterojunctions were synthesized by a facile solvothermal route.The resultant materials were examined by X-ray photoelectron spectrometer(XPS),X-ray diffraction(XRD),scanning electron microscopy(SEM),energy dispersive X-ray spectroscopy(EDX),transmission electron microscopy(TEM),high-resolution transmission electron microscopy(HRTEM),photoluminescence spectroscopy(PL),Fourier transform infrared spectroscopy(FT-IR),UV-Vis diffuse reflection spectroscopy(UV-vis DRS),photocurrent density,electrochemical impedance spectroscopy(EIS),and Brunauer–Emmett–Teller(BET)analyses.After the integration of Fe-MOF with GCN-NSh/Bi_(5)O_(7)Br,the removal constant of tetracycline over the optimal GCN-NSh/Bi_(5)O_(7)Br/Fe-MOF(15wt%)nanocomposite was promoted 33 times compared with that of the pristine GCN.The GCN-NSh/Bi_(5)O_(7)Br/Fe-MOF(15wt%)nanocomposite showed superior photoactivity to azithromycin,metronidazole,and cephalexin removal that was 36.4,20.2,and 14.6 times higher than that of pure GCN,respectively.Radical quenching tests showed that·O_(2)-and h+mainly contributed to the elimination reaction.In addition,the nanocomposite maintained excellent activity after 4 successive cycles.Based on the developed n–n heterojunctions among n-GCN-NSh,n-Bi_(5)O_(7)Br,and n-Fe-MOF semiconductors,the double S-scheme charge transfer mechanism was proposed for the destruction of the selected antibiotics.展开更多
基金financially supported by the National Natural Science Foundation of China (Nos.U2002212,52102058,52204414,52204413,and 52204412)the National Key R&D Program of China (Nos.2021YFC1910504,2019YFC1907101,2019YFC1907103,and 2017YFB0702304)+7 种基金the Key R&D Program of Ningxia Hui Autonomous Region,China (Nos.2021BEG01003 and2020BCE01001)the Xijiang Innovation and Entrepreneurship Team,China (No.2017A0109004)the Macao Young Scholars Program (No.AM2022024),Chinathe Beijing Natural Science Foundation (Nos.L212020 and 2214073),Chinathe Guangdong Basic and Applied Basic Research Foundation,China (Nos.2021A1515110998 and 2020A1515110408)the China Postdoctoral Science Foundation (No.2022M710349)the Fundamental Research Funds for the Central Universities,China (Nos.FRF-BD-20-24A,FRF-TP-20-031A1,FRF-IC-19-017Z,and 06500141)the Integration of Green Key Process Systems MIIT and Scientific and Technological Innovation Foundation of Foshan,China(Nos.BK22BE001 and BK21BE002)。
文摘Exclusive responsiveness to ultraviolet light (~3.2 eV) and high photogenerated charge recombination rate are the two primary drawbacks of pure TiO_(2). We combined N-doped graphene quantum dots (N-GQDs), morphology regulation, and heterojunction construction strategies to synthesize N-GQD/N-doped TiO_(2)/P-doped porous hollow g-C_(3)N_(4) nanotube (PCN) composite photocatalysts (denoted as G-TPCN). The optimal sample (G-TPCN doped with 0.1wt% N-GQD, denoted as 0.1% G-TPCN) exhibits significantly enhanced photoabsorption, which is attributed to the change in bandgap caused by elemental doping (P and N), the improved light-harvesting resulting from the tube structure, and the upconversion effect of N-GQDs. In addition, the internal charge separation and transfer capability of0.1% G-TPCN are dramatically boosted, and its carrier concentration is 3.7, 2.3, and 1.9 times that of N-TiO_(2), PCN, and N-TiO_(2)/PCN(TPCN-1), respectively. This phenomenon is attributed to the formation of Z-scheme heterojunction between N-TiO_(2) and PCNs, the excellent electron conduction ability of N-GQDs, and the short transfer distance caused by the porous nanotube structure. Compared with those of N-TiO_(2), PCNs, and TPCN-1, the H2 production activity of 0.1%G-TPCN under visible light is enhanced by 12.4, 2.3, and 1.4times, respectively, and its ciprofloxacin (CIP) degradation rate is increased by 7.9, 5.7, and 2.9 times, respectively. The optimized performance benefits from excellent photoresponsiveness and improved carrier separation and migration efficiencies. Finally, the photocatalytic mechanism of 0.1% G-TPCN and five possible degradation pathways of CIP are proposed. This study clarifies the mechanism of multiple modification strategies to synergistically improve the photocatalytic performance of 0.1% G-TPCN and provides a potential strategy for rationally designing novel photocatalysts for environmental remediation and solar energy conversion.
基金funded by the National Natural Science Foundation of China(22078138)the“Thousand Talents Plan”of Jiangxi Province(Jxsq2018101018)key projects of the Natural Science Foundation of Jiangxi Province(20202ACBL203009).
文摘Visible-light-driven photocatalysis is a promising technology for the treatment of dye wastewater.In this work,a novel photocatalyst of K-doped g-C_(3)N_(4) loaded on magnetic attapulgite(ATP)(Kω-g-C_(3)N_(4)@ATP-Fe_(3)O_(4))with excellent visible light photocatalytic properties and stability were successfully prepared and characterized.The removal efficiency of Kω-g-C_(3)N_(4)@ATP-Fe_(3)O_(4) for malachite green(MG)was studied,and the degradation mechanism was analyzed and proposed.It was found that the K_(5)-g-C_(3)N_(4)@ATP-Fe_(3)O_(4) photocatalyst possessed excellent degradation efficiency of over 98.0%for the MG dye wastewater under optimal conditions.Moreover,the K_(5)-g-C_(3)N_(4)@ATP-Fe_(3)O_(4) materials possessed good recyclability with a removal rate over 82%after 4 cycles.Under visible light condition,the K_(5)-g-C_(3)N_(4)@ATP-Fe_(3)O_(4) photocatalyst produce radicals of·OH and O_(2)^(-)to degrade the MG dyes,which was supported by electron paramagnetic resonance(EPR)and radical trapping experiments.In addition,the LC-MS analysis interpreted the degradation pathways and intermediates of MG in the solution.The findings in this work indicate that the prepared photocatalytic material has excellent degradation efficiency for MG and can be applied in dye wastewater treatment.
基金supported by the National Natural Science Foundation of China(21875118,22111530112)the support from the Smart Sensing Interdisciplinary Science Center,Nankai University。
文摘Photocatalysis driven by abundant yet intermittent solar energy has considerable potential in renewable energy generation and environmental remediation.The outstanding electronic structure and physicochemical properties of graphitic carbon nitride(g-C_(3)N_(4)),together with unique metal-free characteristic,make them ideal candidates for advanced photocatalysts construction.This review summarizes the up-to-date advances on g-C_(3)N_(4)based photocatalysts from ingenious-design strategies and diversified photocatalytic applications.Notably,the advantages,fabrication methods and limitations of each design strategy are systemically analyzed.In order to deeply comprehend the inner connection of theory–structure–performance upon g-C_(3)N_(4)based photocatalysts,structure/composition designs,corresponding photocatalytic activities and reaction mechanisms are jointly discussed,associated with introducing their photocatalytic applications toward water splitting,carbon dioxide/nitrogen reduction and pollutants degradation,etc.Finally,the current challenges and future perspectives for g-C_(3)N_(4)based materials for photocatalysis are briefly proposed.These design strategies and limitations are also instructive for constructing g-C_(3)N_(4) based materials in other energy and environment-related applications.
基金Jiangsu University of Science and Technology for providing financial support under the Research start-up fund for the introduction of young talent at Jiangsu University of Science and Technology (Grant no. 1112932205)High-level Talents Program of Shihezi University (RCZK2021B25)。
文摘In this research study, we have synthesized the bio-capped ZnO/g-C_(3)N_(4) nanocomposites by employing lemon juice(Citrus limon) as a stabilizer and mediator. Fruitfully, lemon juice which contains various acidic functional groups and citric acid has the capability to block the surface of g-C_(3)N_(4) from chemical reactivity and activated the surface of g-C_(3)N_(4) for various reactions. Consequently, the agglomeration behavior and controlled shape of g-C_(3)N_(4) has also been achieved. Our experimental results i.e. XRD,TEM, HRTEM, PL, FS, XPS, and PEC have confirmed that the lemon juice mediated and green g-C_(3)N_(4)(L-CN) have good performances and remarkable visible light photocatalytic activities as compared to the chemically synthesized g-C_(3)N_(4)(CN). Furthermore, the small surface area and low charge separation of g-C_(3)N_(4) is upgraded by coupling with Zn O nanoparticles. It is proved that the coupling of Zn O worked as a facilitator and photoelectron modulator to enhance the charge separation of g-C_(3)N_(4). Compared to pristine lemon-mediated green g-C_(3)N_(4)(L-CN), the most active sample 5Zn O/L-CN showed ~ 5-fold improvement in activities for ciprofloxacin(CIP) and methylene blue(MB) degradation. More specifically,the mineralization process and degradation pathways, and the mineralization process of ciprofloxacin(CIP) and methylene blue(MB) are suggested. Finally, our present novel research work will provide new access to synthesize the eco-friendly and bio-caped green g-C_(3)N_(4)nanomaterials and their employment for pollutants degradation and environmental purification.
文摘Novel graphitic carbon nitride(g-C_(3)N_(4))nanosheet/Bi_(5)O_(7)Br/NH_(2)-MIL-88B(Fe)photocatalysts(denoted as GCN-NSh/Bi_(5)O_(7)Br/FeMOF,in which MOF is metal–organic framework)with double S-scheme heterojunctions were synthesized by a facile solvothermal route.The resultant materials were examined by X-ray photoelectron spectrometer(XPS),X-ray diffraction(XRD),scanning electron microscopy(SEM),energy dispersive X-ray spectroscopy(EDX),transmission electron microscopy(TEM),high-resolution transmission electron microscopy(HRTEM),photoluminescence spectroscopy(PL),Fourier transform infrared spectroscopy(FT-IR),UV-Vis diffuse reflection spectroscopy(UV-vis DRS),photocurrent density,electrochemical impedance spectroscopy(EIS),and Brunauer–Emmett–Teller(BET)analyses.After the integration of Fe-MOF with GCN-NSh/Bi_(5)O_(7)Br,the removal constant of tetracycline over the optimal GCN-NSh/Bi_(5)O_(7)Br/Fe-MOF(15wt%)nanocomposite was promoted 33 times compared with that of the pristine GCN.The GCN-NSh/Bi_(5)O_(7)Br/Fe-MOF(15wt%)nanocomposite showed superior photoactivity to azithromycin,metronidazole,and cephalexin removal that was 36.4,20.2,and 14.6 times higher than that of pure GCN,respectively.Radical quenching tests showed that·O_(2)-and h+mainly contributed to the elimination reaction.In addition,the nanocomposite maintained excellent activity after 4 successive cycles.Based on the developed n–n heterojunctions among n-GCN-NSh,n-Bi_(5)O_(7)Br,and n-Fe-MOF semiconductors,the double S-scheme charge transfer mechanism was proposed for the destruction of the selected antibiotics.
