Efficient removal of antibiotics is of great significance for the sustainability of aquatic ecosystems.In this work,a new polyoxometalate-based metal-organic hybrid material[Ag_(3)L_(0.5)(HSiW_(12)O_(4)0)]·2C_(2)...Efficient removal of antibiotics is of great significance for the sustainability of aquatic ecosystems.In this work,a new polyoxometalate-based metal-organic hybrid material[Ag_(3)L_(0.5)(HSiW_(12)O_(4)0)]·2C_(2)H_(5)OH·2CH_(3)CN(Ag-L-SiW_(12))was prepared by using Keggin-type polyoxometalate anion and thiacalix[4]arene-based ligand(L)via solvothermal method.Subsequently,a composite heterojunction Ag-L-SiW_(12)@BiVO_(4)photoanode was fabricated by loading Ag-L-SiW_(12)on the surface of BiVO_(4).The photoelectrocatalytic degradation performance of ciprofloxacin(CIP)was explored under the simulated solar radiation.Remarkably,the CIP degradation efficiency reached 93%within 240 min using the optimal Ag-LSiW_(12)@BiVO_(4)photoanode,which is approximately 2 and 23 times those of pristine BiVO_(4)and Ag-L-SiW_(12),respectively.Furthermore,density functional theory(DFT)calculations were conducted to elucidate the role of Ag-L-SiW_(12)during the photoelectrocatalytic process.This work offers an example of the efficient composite photoelectrocatalysts for the treatment of antibiotic wastewater.展开更多
Growing attention to the development of sustainable solar-to-energy conversion applications has resulted in the synthesis of promising and environment-friendly nanomaterials as energy harvesters.Among various carbon n...Growing attention to the development of sustainable solar-to-energy conversion applications has resulted in the synthesis of promising and environment-friendly nanomaterials as energy harvesters.Among various carbon nanomaterials,carbon dots(CDs)have received significant attention due to their excellent light absorption capability,broad absorption region,and superior photostability with enormous potential for solar energy applications.Therefore,utilizing and modulating the charge carriers generated from CDs is critical for achieving a high energy conversion efficiency of CDs.Herein,we focus on the distinct characteristics of CDs as energy converters from charge excitation to charge separation and transfer for various solar-to-energy applications,including photovoltaic cells,photocatalysts,and photoelectrocatalysts.We anticipate that this review will offer insight into the synthesis and design of novel nanocomposites with a fundamental analysis of the photochemical properties and future development of energy conversion devices.展开更多
The influence of an externally applied bias on photocatalytic performance of crystallized TiO2/Ti nanotubular electrode formed by anodization in fluoride-based electrolyte were investigated and compared to the behavio...The influence of an externally applied bias on photocatalytic performance of crystallized TiO2/Ti nanotubular electrode formed by anodization in fluoride-based electrolyte were investigated and compared to the behavior of multiporous TiO2 electrode. The photoelectrocatalytic oxidation behavior of methanol over the nanotubular electrode has been studied by measuring photocurrent response, potentiodynamic polarization spectroscopy and using electrochemical impedance spectroscopy （EIS）. It was found that the photoelectrocatalytic oxida- tion and the charge transfer rate constant of reaction on TiO2/Ti nanotubular electrode can significantly be increased by applying electrochemical bias. Moreover, TiO2 electrodes have considerably better performance alytic performance. based on the results, it was found that the nanotubular in comparison with porous samples in photoelectrocatalytic performance.展开更多
As a new member of the carbon family,graphdiyne is an intrinsic semiconductor featuring a natural bandgap,which endues it potential for direct application in photoelectric devices.However,without cooperating with othe...As a new member of the carbon family,graphdiyne is an intrinsic semiconductor featuring a natural bandgap,which endues it potential for direct application in photoelectric devices.However,without cooperating with other active materials,conventional hexacetylene-benzene graphdiyne(HEB-GDY)shows poor performances in photocatalysis and photoelectric devices due to its non-ideal visible light absorption,low separation efficiency of the photogenerated carriers and insufficient sites for hydrogen production.Herein,we report a molecular engineering strategy for the regulation of GDY-based carbon materials,by incorporating a strong pyrene absorption group into the matrix of graphdiyne,to obtain pyrenyl graphdiyne(Pyr-GDY)nanofibers through a modified Glaser-Hay coupling reaction of 1,3,6,8-tetraethynylpyrene(TEP)monomers.For comparison,phenyl graphdiyne(Phe-GDY)nanosheets were also constructed using 1,3,4,6-tetraethynylbenzene(TEB)as a monomer.Compared with Phe-GDY,Pyr-GDY exhibits a wider visible light absorption band,promoted efficiency of the charge separation/transport and more sufficient active sites for water reduction.As a result,Pyr-GDY alone displays superior photoelectrocatalytic performance for water splitting,giving a cathode photocurrent density of^138μA cm-2 at a potential of-0.1 Vversus normal hydrogen electrode(NHE)in neutral aqueous solution,which is almost ten and twelve times as high as those of Phe-GDY(14μA cm-2)and HEB-GDY(12μA cm-2),respectively.Such a performance is also superior to those of most reported carbonbased metal-free photocathode.The results of theoretical calculations reveal that the carbon atoms in the acetylene bonds are the active sites for proton reduction.This work offers a new strategy for the construction of graphdiyne-based metal-free photoelectrocatalysts with enhanced photoelectrocatalytic performance.展开更多
In an era of graphene-based nanomaterials as the most widely studied two-dimensional (2D) materials for enhanced performance of devices and systems in solar energy conversion applications, molybdenum disulfide (MoS2) ...In an era of graphene-based nanomaterials as the most widely studied two-dimensional (2D) materials for enhanced performance of devices and systems in solar energy conversion applications, molybdenum disulfide (MoS2) stands out as a promising alternative 2D material with excellent properties. This review first examined various methods for MoS2 synthesis. It, then, summarized the unique structure and properties of MoS2 nanosheets. Finally, it presented the latest advances in the use of M0S2 nanosheets for important solar energy applications, including solar thermal water purification, photocatalytic process, and photoelectrocatalytic process.展开更多
基金supported by the National Natural Science Foundation of China(Grant No.21471029).
文摘Efficient removal of antibiotics is of great significance for the sustainability of aquatic ecosystems.In this work,a new polyoxometalate-based metal-organic hybrid material[Ag_(3)L_(0.5)(HSiW_(12)O_(4)0)]·2C_(2)H_(5)OH·2CH_(3)CN(Ag-L-SiW_(12))was prepared by using Keggin-type polyoxometalate anion and thiacalix[4]arene-based ligand(L)via solvothermal method.Subsequently,a composite heterojunction Ag-L-SiW_(12)@BiVO_(4)photoanode was fabricated by loading Ag-L-SiW_(12)on the surface of BiVO_(4).The photoelectrocatalytic degradation performance of ciprofloxacin(CIP)was explored under the simulated solar radiation.Remarkably,the CIP degradation efficiency reached 93%within 240 min using the optimal Ag-LSiW_(12)@BiVO_(4)photoanode,which is approximately 2 and 23 times those of pristine BiVO_(4)and Ag-L-SiW_(12),respectively.Furthermore,density functional theory(DFT)calculations were conducted to elucidate the role of Ag-L-SiW_(12)during the photoelectrocatalytic process.This work offers an example of the efficient composite photoelectrocatalysts for the treatment of antibiotic wastewater.
基金National Research Foundation of Korea,Grant/Award Numbers:NRF-2017M3A7B4052802,NRF-2018R1A5A1025208。
文摘Growing attention to the development of sustainable solar-to-energy conversion applications has resulted in the synthesis of promising and environment-friendly nanomaterials as energy harvesters.Among various carbon nanomaterials,carbon dots(CDs)have received significant attention due to their excellent light absorption capability,broad absorption region,and superior photostability with enormous potential for solar energy applications.Therefore,utilizing and modulating the charge carriers generated from CDs is critical for achieving a high energy conversion efficiency of CDs.Herein,we focus on the distinct characteristics of CDs as energy converters from charge excitation to charge separation and transfer for various solar-to-energy applications,including photovoltaic cells,photocatalysts,and photoelectrocatalysts.We anticipate that this review will offer insight into the synthesis and design of novel nanocomposites with a fundamental analysis of the photochemical properties and future development of energy conversion devices.
文摘The influence of an externally applied bias on photocatalytic performance of crystallized TiO2/Ti nanotubular electrode formed by anodization in fluoride-based electrolyte were investigated and compared to the behavior of multiporous TiO2 electrode. The photoelectrocatalytic oxidation behavior of methanol over the nanotubular electrode has been studied by measuring photocurrent response, potentiodynamic polarization spectroscopy and using electrochemical impedance spectroscopy （EIS）. It was found that the photoelectrocatalytic oxida- tion and the charge transfer rate constant of reaction on TiO2/Ti nanotubular electrode can significantly be increased by applying electrochemical bias. Moreover, TiO2 electrodes have considerably better performance alytic performance. based on the results, it was found that the nanotubular in comparison with porous samples in photoelectrocatalytic performance.
基金This work was supported by the National Natural Science Foundation of China(No.21571119)the Applied Basic Research Project of Shanxi Province(No.201901D211393 and No.201901D211398)+1 种基金Scientific and Technological Innovation Programs of Higher Education Institution in Shanxi(No.2019L0466)1331 Engineering of Shanxi Province.
基金supported by the National Key R&D Program of China(2017YFA0700104)the National Natural Science Foundation of China(21790052,21702146,21805207)111 Project of China(D17003)。
文摘As a new member of the carbon family,graphdiyne is an intrinsic semiconductor featuring a natural bandgap,which endues it potential for direct application in photoelectric devices.However,without cooperating with other active materials,conventional hexacetylene-benzene graphdiyne(HEB-GDY)shows poor performances in photocatalysis and photoelectric devices due to its non-ideal visible light absorption,low separation efficiency of the photogenerated carriers and insufficient sites for hydrogen production.Herein,we report a molecular engineering strategy for the regulation of GDY-based carbon materials,by incorporating a strong pyrene absorption group into the matrix of graphdiyne,to obtain pyrenyl graphdiyne(Pyr-GDY)nanofibers through a modified Glaser-Hay coupling reaction of 1,3,6,8-tetraethynylpyrene(TEP)monomers.For comparison,phenyl graphdiyne(Phe-GDY)nanosheets were also constructed using 1,3,4,6-tetraethynylbenzene(TEB)as a monomer.Compared with Phe-GDY,Pyr-GDY exhibits a wider visible light absorption band,promoted efficiency of the charge separation/transport and more sufficient active sites for water reduction.As a result,Pyr-GDY alone displays superior photoelectrocatalytic performance for water splitting,giving a cathode photocurrent density of^138μA cm-2 at a potential of-0.1 Vversus normal hydrogen electrode(NHE)in neutral aqueous solution,which is almost ten and twelve times as high as those of Phe-GDY(14μA cm-2)and HEB-GDY(12μA cm-2),respectively.Such a performance is also superior to those of most reported carbonbased metal-free photocathode.The results of theoretical calculations reveal that the carbon atoms in the acetylene bonds are the active sites for proton reduction.This work offers a new strategy for the construction of graphdiyne-based metal-free photoelectrocatalysts with enhanced photoelectrocatalytic performance.
文摘In an era of graphene-based nanomaterials as the most widely studied two-dimensional (2D) materials for enhanced performance of devices and systems in solar energy conversion applications, molybdenum disulfide (MoS2) stands out as a promising alternative 2D material with excellent properties. This review first examined various methods for MoS2 synthesis. It, then, summarized the unique structure and properties of MoS2 nanosheets. Finally, it presented the latest advances in the use of M0S2 nanosheets for important solar energy applications, including solar thermal water purification, photocatalytic process, and photoelectrocatalytic process.
