The rapid recombination of photogenerated carriers poses a significant limitation on the use of CdS quantum dots(QDs)in photocatalysis.Herein,the construction of a novel S-scheme heterojunction between cubic-phase CdS...The rapid recombination of photogenerated carriers poses a significant limitation on the use of CdS quantum dots(QDs)in photocatalysis.Herein,the construction of a novel S-scheme heterojunction between cubic-phase CdS QDs and hollow nanotube In_(2)O_(3)is successfully achieved using an electrostatic self-assembly method.Under visible light irradiation,all CdS-In_(2)O_(3)composites exhibit higher hydrogen evolution efficiency compared to pure CdS QDs.Notably,the photocatalytic H_(2)evolution rate of the optimal CdS-7%In_(2)O_(3)composite is determined to be 2258.59μmol g^(−1)h^(−1),approximately 12.3 times higher than that of pure CdS.The cyclic test indicates that the CdS-In_(2)O_(3)composite maintains considerable activity even after 5 cycles,indicating its excellent stability.In situ X-ray photoelectron spectroscopy and density functional theory calculations confirm that carrier migration in CdS-In_(2)O_(3)composites adheres to a typical S-scheme heterojunction mechanism.Additionally,a series of characterizations demonstrate that the formation of S-scheme heterojunctions between In_(2)O_(3)and CdS inhibits charge recombination and accelerates the separation and migration of photogenerated carriers in the CdS QDs,thus achieving enhanced photocatalytic performance.This work elucidates the pivotal role of S-scheme heterojunctions in photocatalytic H_(2)production and offers novel insights into the construction of effective composite photocatalysts.展开更多
A deficiency ofγδT cells has been described in Crohn's disease(CD).AIM To analyze the gene expression of interleukin 7(IL-7)and its receptors in the tissues of patients with CD.METHODS We studied the peripheral ...A deficiency ofγδT cells has been described in Crohn's disease(CD).AIM To analyze the gene expression of interleukin 7(IL-7)and its receptors in the tissues of patients with CD.METHODS We studied the peripheral blood of 80 patients with CD,comparing them with a group of 80 healthy subjects.The number and apoptosis ofαβandγδT cells in peripheral blood and the proportion ofαβandγδT cells in the intestinal tissues of patients with CD(n=25)were studied.The gene and protein expression of IL-7,IL-2 receptor subunitγ[cluster of differentiation 132(CD132)],receptorα(CD127),and caspase-3 in tissues was analyzed by quantitative PCR.Serum IL-7 levels were also analyzed.RESULTS In patients with CD,a decreased number ofγδT cells and an increase in the apoptosis of CD56+αβandγδT cells in peripheral blood was observed(P<0.0001 and P<0.01)respectively,and there was an inverse correlation among T subsets and their apoptosis.In addition,IL-7 gene expression and IL-7 protein in the tissues of these patients were increased.The titers of caspase-3 in tissues were low vs control group(P>0.01).The percentage of CD8+γδT cells decreased in tissues(P<0.01),and was directly related to IL-7 levels in peripheral blood.The expression of IL-2 receptor subunitγ(CD132)was greatly decreased in the tissues of patients with CD(P<0.05).CONCLUSION There may be a cause-effect relationship between the lower gene expression of the IL-2 receptor subunitγ(CD132)in tissues of patients with CD andγδT cells immunodeficiency.展开更多
The Bi2S3,CdS and Bi2S3/CdS photocatalysts were prepared by direct reactions between their corresponding salt and thiourea in a hy- drothermal autoclave.The photocatalytic activities of these photocatalysts for reduci...The Bi2S3,CdS and Bi2S3/CdS photocatalysts were prepared by direct reactions between their corresponding salt and thiourea in a hy- drothermal autoclave.The photocatalytic activities of these photocatalysts for reducing CO2 to CH3OH under visible light irradiation have been investigated.The results show that the photocatalytic activity and visible light response of Bi2S3 are higher than those of CdS.The Bi2S3 modification can enhance the photocatalytic activity and visible light response of CdS.The photocatalytic activity of Bi2S3/CdS hetero-junction photocatalyst was the highest and the highest yields of methanol was 613μmol/g when the weight proportion of Bi2S3 to CdS was 15%,which was about three times as large as that of CdS or two times of that of Bi2S3.展开更多
The rapid recombination of photo-generated electron-hole pairs,insufficient active sites,and strong photocorrosion have considerably restricted the practical application of Cd S in photocatalytic fields.Herein,we desi...The rapid recombination of photo-generated electron-hole pairs,insufficient active sites,and strong photocorrosion have considerably restricted the practical application of Cd S in photocatalytic fields.Herein,we designed and constructed a 2D/2D/2D layered heterojunction photocatalyst with cascaded 2D coupling interfaces.Experiments using electron spin resonance spectroscopy,ultraviolet photoelectron spectroscopy,and in-situ irradiation X-ray photoelectron spectroscopy were conducted to confirm the 2D layered CdS/WO_(3) step-scheme(S-scheme)heterojunctions and CdS/MX ohmic junctions.Impressively,it was found that the strong interfacial electric fields in the S-scheme heterojunction photocatalysts could effectively promote spatially directional charge separation and transport between CdS and WO_(3) nanosheets.In addition,2D Ti_(3)C_(2) MXene nanosheets with a smaller work function and excellent metal conductivity when used as a co-catalyst could build ohmic junctions with Cd S nanosheets,thus providing a greater number of electron transfer pathways and hydrogen evolution sites.Results showed that the highest visible-light hydrogen evolution rate of the optimized MX-Cd S/WO_(3) layered multi-heterostructures could reach as high as 27.5 mmol/g/h,which was 11.0 times higher than that of pure CdS nanosheets.Notably,the apparent quantum efficiency reached 12.0% at 450 nm.It is hoped that this study offers a reliable approach for developing multifunctional photocatalysts by integrating S-scheme and ohmic-junction built-in electric fields and rationally designing a 2D/2D interface for efficient light-to-hydrogen fuel production.展开更多
Novel CdS and Bi2S3 hollow nanospheres were prepared by simple “one-pot” biomolecule-assisted hydrothermal method using glutathione (GSH) as sulfur source and structure-directing reagents. The single-phase CdS and B...Novel CdS and Bi2S3 hollow nanospheres were prepared by simple “one-pot” biomolecule-assisted hydrothermal method using glutathione (GSH) as sulfur source and structure-directing reagents. The single-phase CdS and Bi2S3 photocatalysts were capable of evolving H2 from aqueous solutions containing a sacrificial electron donor, under visible light irradiation (λ ≥ 420 nm) with Pt co-catalyst. A possible formation mechanism of complexation, S-C bond rupture, and spherical aggregate followed isotropic Ostwal ripening or anisotropic Ostwal ripening was proposed in this study.展开更多
The development of low-cost semiconductor photocatalysts for highly efficient and durable photocatalytic H2 evolution under visible light is very challenging.In this study,we combine low-cost metallic Ni3C cocatalysts...The development of low-cost semiconductor photocatalysts for highly efficient and durable photocatalytic H2 evolution under visible light is very challenging.In this study,we combine low-cost metallic Ni3C cocatalysts with twin nanocrystal Zn0.5Cd0.5S(ZCS)solid solution homojunctions for an efficient visible-light-driven H2 production by a simple approach.As-synthesized Zn0.5Cd0.5S-1%Ni3C(ZCS-1)heterojunction/homojunction nanohybrid exhibited the highest photocatalytic H2-evolution rate of 783μmol h‒1 under visible light,which is 2.88 times higher than that of pristine twin nanocrystal ZCS solid solution.The apparent quantum efficiencies of ZCS and ZCS-1 are measured to be 6.13%and 19.25%at 420 nm,respectively.Specifically,the homojunctions between the zinc blende and wurtzite segments in twin nanocrystal ZCS solid solution can significantly improve the light absorption and separation of photogenerated electron-hole pairs.Furthermore,the heterojunction between ZCS and metallic Ni3C NP cocatalysts can efficiently trap excited electrons from ZCS solid solution and enhance the H2-evolution kinetics at the surface for improving catalytic activity.This study demonstrates a unique one-step strategy for constructing heterojunction/homojunction hybrid nanostructures for a more efficient photocatalytic H2 evolution compared to other noble metal photocatalytic systems.展开更多
The band alignment at the front interfaces is crucial for the performance of Sb_(2)Se_(3) solar cell with superstrate configuration.Herein,a Sn O_(2)/Ti O_(2) thin film,demonstrated beneficial for carrier transport in...The band alignment at the front interfaces is crucial for the performance of Sb_(2)Se_(3) solar cell with superstrate configuration.Herein,a Sn O_(2)/Ti O_(2) thin film,demonstrated beneficial for carrier transport in Sb_(2)Se_(3) device by the first-principle calculation and experiment,is proposed to reduce the parasitic absorption caused by CdS and optimize the band alignment of Sb_(2)Se_(3) solar cell.Thanks to the desirable transmittance of SnO_(2)/TiO_(2) layer,the Sb_(2)Se_(3) solar cell with SnO_(2)/TiO_(2)/(CdS-38 nm) electron transport layer performances better than (CdS-70 nm)/Sb_(2)Se_(3) solar cell.The optimized band alignment,the reduced interface defects and the decreased current leakage of Sb_(2)Se_(3) solar cell enable the short-circuit current density,fill factor,open-circuit voltage and efficiency of the Sb_(2)Se_(3) solar cell increase by 26.7%,112%,33.1%and 250%respectively when comparing with TiO_(2)/Sb_(2)Se_(3) solar cell without modification.Finally,an easily prepared Sn O_(2)/Ti O_(2)/CdS ETL is successfully applied on Sb_(2)Se_(3) solar cell by the first time and contributes to the best efficiency of 7.0%in this work,which is remarkable for Sb_(2)Se_(3) solar cells free of hole transporting materials and toxic CdCl_(2) treatment.This work is expected to provide a valuable reference for future ETL design and band alignment for Sb_(2)Se_(3) solar cell and other optoelectronic devices.展开更多
Cadmium sulfide(CdS)is an n-type semiconductor with excellent electrical conductivity that is widely used as an electron transport material(ETM)in solar cells.At present,numerous methods for preparing CdS thin films h...Cadmium sulfide(CdS)is an n-type semiconductor with excellent electrical conductivity that is widely used as an electron transport material(ETM)in solar cells.At present,numerous methods for preparing CdS thin films have emerged,among which magnetron sputtering(MS)is one of the most commonly used vacuum techniques.For this type of technique,the substrate temperature is one of the key deposition parameters that affects the interfacial properties between the target film and substrate,determining the specific growth habits of the films.Herein,the effect of substrate temperature on the microstructure and electrical properties of magnetron-sputtered CdS(MS-CdS)films was studied and applied for the first time in hydrothermally deposited antimony selenosulfide(Sb_(2)(S,Se)_(3))solar cells.Adjusting the substrate temperature not only results in the design of the flat and dense film with enhanced crystallinity but also leads to the formation of an energy level arrangement with a Sb_(2)(S,Se)_(3)layer that is more favorable for electron transfer.In addition,we developed an oxygen plasma treatment for CdS,reducing the parasitic absorption of the device and resulting in an increase in the short-circuit current density of the solar cell.This study demonstrates the feasibility of MS-CdS in the fabrication of hydrothermal Sb_(2)(S,Se)_(3)solar cells and provides interface optimization strategies to improve device performance.展开更多
For a long time, there has been global concern over the environment and energy problems. Recently, the problems, which have brought about serious effect on the global living condition, have been in the ‘‘spotlight&q...For a long time, there has been global concern over the environment and energy problems. Recently, the problems, which have brought about serious effect on the global living condition, have been in the ‘‘spotlight" and given impetus to the universal's efforts to head for the same direction: stem the worst warming and strive for the renewable energy source. Hydrogen peroxide(H_2O_2) is undoubtedly a good choice,which holds the promise as a clean, efficient, safe and transferrable energy carrier. Octahedral coordination polymer, Cd_3(C_3N_3S_3)_2, was found to be a robust photocatalyst for H_2O_2 generation under visible light irradiation. To further improve the H_2O_2 generation efficiency, adhering the octahedron to reduced graphene(rGO) was applied as the strategy herein. The study shows that by adhering Cd_3(C_3N_3S_3)_2to rGO, the formation of H_2O_2 is 2.5-fold enhanced and its deformation is concurrently suppressed. This work not only demonstrates the effectiveness of adhering Cd_3(C_3N_3S_3)_2polymer to rGO for the improvement of the polymer's photocatalytic performance, but also proposes a general way for the fabrication of graphene/coordination compound hybrids for maximizing their synergy.展开更多
The production of renewable fossil fuels such as CH_(4) and CO by photocatalytic CO_(2)reduction has attracted more and more attention.However,single photocatalyst is less efficient for photocatalytic reduction of CO_...The production of renewable fossil fuels such as CH_(4) and CO by photocatalytic CO_(2)reduction has attracted more and more attention.However,single photocatalyst is less efficient for photocatalytic reduction of CO_(2)due to the fast recombination of photogenerated electron pairs.Herein,we successfully prepare CdS-Ag_(2)S composite by assembling the Ag_(2)S QDs cocatalyst on the surface of CdS nanosheet-assembled flower through oil-bath solvothermal method.This composite is prepared through a simple self-assembly strategy using cadmium chloride,ammonia and thiourea as precursors of the CdS nanosheet-assembled flower and silver nitrate and 3-mercaptopropionic acid as the precursors of Ag_(2)S QDs.The average diameter of Ag_(2)S QDs is apparently 6.0 nm.The light absorption edge of the composite is at around 560 nm,with the corresponding band gap at 2.14 eV.The CdS-Ag_(2)S QDs composite with 5 wt%Ag_(2)S QDs loaded achieves CO evolution rate of 16.6μmol·g^(-1)·h^(-1)without noble-metal cocatalysts.This strengthened photocatalytic performance and photocatalytic stability were attributed to the energy band broadening of Ag_(2)S QDs caused by quantum size effect and the large specific surface area due to the assembled flower.The mechanism underlying the enhanced photocatalytic CO_(2)reduction activity is further proposed.This study demonstrates that semiconductor-based quantum dots are strong candidates for excellent cocatalysts in photocatalysis.展开更多
Recombinant interleukin-33(IL-33)inhibits tumor growth,but the detailed immunological mechanism is still unknown.IL-33-mediated tumor suppression did not occur in Batf3^(−/−)mice,indicating that conventional type 1 de...Recombinant interleukin-33(IL-33)inhibits tumor growth,but the detailed immunological mechanism is still unknown.IL-33-mediated tumor suppression did not occur in Batf3^(−/−)mice,indicating that conventional type 1 dendritic cells(cDC1s)play a key role in IL-33-mediated antitumor immunity.A population of CD103^(+)cDC1s,which were barely detectable in the spleens of normal mice,increased significantly in the spleens of IL-33-treated mice.The newly emerged splenic CD103^(+)cDC1s were distinct from conventional splenic cDC1s based on their spleen residency,robust effector T-cell priming ability,and surface expression of FCGR3.DCs and DC precursors did not express Suppressor of Tumorigenicity 2(ST2).However,recombinant IL-33 induced spleen-resident FCGR3^(+)CD103^(+)cDC1s,which were found to be differentiated from DC precursors by bystander ST2+immune cells.Through immune cell fractionation and depletion assays,we found that IL-33-primed ST2^(+)basophils play a crucial role in the development of FCGR3^(+)CD103^(+)cDC1s by secreting IL-33-driven extrinsic factors.Recombinant GM-CSF also induced the population of CD103^(+)cDC1s,but the population neither expressed FCGR3 nor induced any discernable antitumor immunity.The population of FCGR3^(+)CD103^(+)cDC1s was also generated in vitro culture of Flt3L-mediated bone marrow-derived DCs(FL-BMDCs)when IL-33 was added in a pre-DC stage of culture.FL-BMDCs generated in the presence of IL-33(FL-33-DCs)offered more potent tumor immunotherapy than control Flt3L-BMDCs(FL-DCs).Human monocyte-derived DCs were also more immunogenic when exposed to IL-33-induced factors.Our findings suggest that recombinant IL-33 or an IL-33-mediated DC vaccine could be an attractive protocol for better tumor immunotherapy.展开更多
Designing photocatalysts with high light utilization and efficient photogenerated carrier separation for pollutant degradation is one of the important topics for sustainable development.In this study,hierarchical core...Designing photocatalysts with high light utilization and efficient photogenerated carrier separation for pollutant degradation is one of the important topics for sustainable development.In this study,hierarchical core–shell materialα-Fe_(2)O_(3)@ZnIn_(2)S_(4)with a step-scheme(S-scheme)heterojunction is synthesized by in situ growth technique,and MXene Ti_(3)C_(2)quantum dots(QDs)are introduced to construct a double-heterojunction tandem mechanism.The photodegradation efficiency ofα-Fe_(2)O_(3)@ZnIn_(2)S_(4)/Ti_(3)C_(2)QDs to bisphenol A is 96.1%and its reaction rate constant attained 0.02595 min^(−1),which is 12.3 times that of pureα-Fe_(2)O_(3).Meanwhile,a series of characterizations analyze the reasons for the enhanced photocatalytic activity,and the charge transport path of the S-scheme heterojunction/Schottky junction tandem is investigated.The construction of the S-scheme heterojunction enables the photo-generated electrons ofα-Fe_(2)O_(3)and the holes of ZnIn2S4 to transfer and combine under the action of the reverse built-in electric field.Due to the metallic conductivity of Ti_(3)C_(2)QDs,the photogenerated electrons of ZnIn_(2)S_(4)are further transferred to Ti_(3)C_(2)QDs to form a Schottky junction,which in turn forms a double-heterojunction tandem mechanism,showing a remarkable charge separation efficiency.This work provides a new opinion for the construction of tandem double heterojunctions to degrade harmful pollutants.展开更多
文摘The rapid recombination of photogenerated carriers poses a significant limitation on the use of CdS quantum dots(QDs)in photocatalysis.Herein,the construction of a novel S-scheme heterojunction between cubic-phase CdS QDs and hollow nanotube In_(2)O_(3)is successfully achieved using an electrostatic self-assembly method.Under visible light irradiation,all CdS-In_(2)O_(3)composites exhibit higher hydrogen evolution efficiency compared to pure CdS QDs.Notably,the photocatalytic H_(2)evolution rate of the optimal CdS-7%In_(2)O_(3)composite is determined to be 2258.59μmol g^(−1)h^(−1),approximately 12.3 times higher than that of pure CdS.The cyclic test indicates that the CdS-In_(2)O_(3)composite maintains considerable activity even after 5 cycles,indicating its excellent stability.In situ X-ray photoelectron spectroscopy and density functional theory calculations confirm that carrier migration in CdS-In_(2)O_(3)composites adheres to a typical S-scheme heterojunction mechanism.Additionally,a series of characterizations demonstrate that the formation of S-scheme heterojunctions between In_(2)O_(3)and CdS inhibits charge recombination and accelerates the separation and migration of photogenerated carriers in the CdS QDs,thus achieving enhanced photocatalytic performance.This work elucidates the pivotal role of S-scheme heterojunctions in photocatalytic H_(2)production and offers novel insights into the construction of effective composite photocatalysts.
文摘A deficiency ofγδT cells has been described in Crohn's disease(CD).AIM To analyze the gene expression of interleukin 7(IL-7)and its receptors in the tissues of patients with CD.METHODS We studied the peripheral blood of 80 patients with CD,comparing them with a group of 80 healthy subjects.The number and apoptosis ofαβandγδT cells in peripheral blood and the proportion ofαβandγδT cells in the intestinal tissues of patients with CD(n=25)were studied.The gene and protein expression of IL-7,IL-2 receptor subunitγ[cluster of differentiation 132(CD132)],receptorα(CD127),and caspase-3 in tissues was analyzed by quantitative PCR.Serum IL-7 levels were also analyzed.RESULTS In patients with CD,a decreased number ofγδT cells and an increase in the apoptosis of CD56+αβandγδT cells in peripheral blood was observed(P<0.0001 and P<0.01)respectively,and there was an inverse correlation among T subsets and their apoptosis.In addition,IL-7 gene expression and IL-7 protein in the tissues of these patients were increased.The titers of caspase-3 in tissues were low vs control group(P>0.01).The percentage of CD8+γδT cells decreased in tissues(P<0.01),and was directly related to IL-7 levels in peripheral blood.The expression of IL-2 receptor subunitγ(CD132)was greatly decreased in the tissues of patients with CD(P<0.05).CONCLUSION There may be a cause-effect relationship between the lower gene expression of the IL-2 receptor subunitγ(CD132)in tissues of patients with CD andγδT cells immunodeficiency.
基金supported by the National Natural Science Foundation of China(No.20906034)the Key Academic Program of the 3rd Phase"211 Project" of South China Agricultural University(No.2009B010100001)China Postdoctoral Science Foundation(No.20080430820)
文摘The Bi2S3,CdS and Bi2S3/CdS photocatalysts were prepared by direct reactions between their corresponding salt and thiourea in a hy- drothermal autoclave.The photocatalytic activities of these photocatalysts for reducing CO2 to CH3OH under visible light irradiation have been investigated.The results show that the photocatalytic activity and visible light response of Bi2S3 are higher than those of CdS.The Bi2S3 modification can enhance the photocatalytic activity and visible light response of CdS.The photocatalytic activity of Bi2S3/CdS hetero-junction photocatalyst was the highest and the highest yields of methanol was 613μmol/g when the weight proportion of Bi2S3 to CdS was 15%,which was about three times as large as that of CdS or two times of that of Bi2S3.
文摘The rapid recombination of photo-generated electron-hole pairs,insufficient active sites,and strong photocorrosion have considerably restricted the practical application of Cd S in photocatalytic fields.Herein,we designed and constructed a 2D/2D/2D layered heterojunction photocatalyst with cascaded 2D coupling interfaces.Experiments using electron spin resonance spectroscopy,ultraviolet photoelectron spectroscopy,and in-situ irradiation X-ray photoelectron spectroscopy were conducted to confirm the 2D layered CdS/WO_(3) step-scheme(S-scheme)heterojunctions and CdS/MX ohmic junctions.Impressively,it was found that the strong interfacial electric fields in the S-scheme heterojunction photocatalysts could effectively promote spatially directional charge separation and transport between CdS and WO_(3) nanosheets.In addition,2D Ti_(3)C_(2) MXene nanosheets with a smaller work function and excellent metal conductivity when used as a co-catalyst could build ohmic junctions with Cd S nanosheets,thus providing a greater number of electron transfer pathways and hydrogen evolution sites.Results showed that the highest visible-light hydrogen evolution rate of the optimized MX-Cd S/WO_(3) layered multi-heterostructures could reach as high as 27.5 mmol/g/h,which was 11.0 times higher than that of pure CdS nanosheets.Notably,the apparent quantum efficiency reached 12.0% at 450 nm.It is hoped that this study offers a reliable approach for developing multifunctional photocatalysts by integrating S-scheme and ohmic-junction built-in electric fields and rationally designing a 2D/2D interface for efficient light-to-hydrogen fuel production.
文摘Novel CdS and Bi2S3 hollow nanospheres were prepared by simple “one-pot” biomolecule-assisted hydrothermal method using glutathione (GSH) as sulfur source and structure-directing reagents. The single-phase CdS and Bi2S3 photocatalysts were capable of evolving H2 from aqueous solutions containing a sacrificial electron donor, under visible light irradiation (λ ≥ 420 nm) with Pt co-catalyst. A possible formation mechanism of complexation, S-C bond rupture, and spherical aggregate followed isotropic Ostwal ripening or anisotropic Ostwal ripening was proposed in this study.
文摘The development of low-cost semiconductor photocatalysts for highly efficient and durable photocatalytic H2 evolution under visible light is very challenging.In this study,we combine low-cost metallic Ni3C cocatalysts with twin nanocrystal Zn0.5Cd0.5S(ZCS)solid solution homojunctions for an efficient visible-light-driven H2 production by a simple approach.As-synthesized Zn0.5Cd0.5S-1%Ni3C(ZCS-1)heterojunction/homojunction nanohybrid exhibited the highest photocatalytic H2-evolution rate of 783μmol h‒1 under visible light,which is 2.88 times higher than that of pristine twin nanocrystal ZCS solid solution.The apparent quantum efficiencies of ZCS and ZCS-1 are measured to be 6.13%and 19.25%at 420 nm,respectively.Specifically,the homojunctions between the zinc blende and wurtzite segments in twin nanocrystal ZCS solid solution can significantly improve the light absorption and separation of photogenerated electron-hole pairs.Furthermore,the heterojunction between ZCS and metallic Ni3C NP cocatalysts can efficiently trap excited electrons from ZCS solid solution and enhance the H2-evolution kinetics at the surface for improving catalytic activity.This study demonstrates a unique one-step strategy for constructing heterojunction/homojunction hybrid nanostructures for a more efficient photocatalytic H2 evolution compared to other noble metal photocatalytic systems.
基金supported by the National Key R&D Program of China(2019YFB1503500)the National Natural Science Foundation of China(U1902218,11774187)the Postgraduate Education Innovation Project of Tianjin,China(2021YJSB002)。
文摘The band alignment at the front interfaces is crucial for the performance of Sb_(2)Se_(3) solar cell with superstrate configuration.Herein,a Sn O_(2)/Ti O_(2) thin film,demonstrated beneficial for carrier transport in Sb_(2)Se_(3) device by the first-principle calculation and experiment,is proposed to reduce the parasitic absorption caused by CdS and optimize the band alignment of Sb_(2)Se_(3) solar cell.Thanks to the desirable transmittance of SnO_(2)/TiO_(2) layer,the Sb_(2)Se_(3) solar cell with SnO_(2)/TiO_(2)/(CdS-38 nm) electron transport layer performances better than (CdS-70 nm)/Sb_(2)Se_(3) solar cell.The optimized band alignment,the reduced interface defects and the decreased current leakage of Sb_(2)Se_(3) solar cell enable the short-circuit current density,fill factor,open-circuit voltage and efficiency of the Sb_(2)Se_(3) solar cell increase by 26.7%,112%,33.1%and 250%respectively when comparing with TiO_(2)/Sb_(2)Se_(3) solar cell without modification.Finally,an easily prepared Sn O_(2)/Ti O_(2)/CdS ETL is successfully applied on Sb_(2)Se_(3) solar cell by the first time and contributes to the best efficiency of 7.0%in this work,which is remarkable for Sb_(2)Se_(3) solar cells free of hole transporting materials and toxic CdCl_(2) treatment.This work is expected to provide a valuable reference for future ETL design and band alignment for Sb_(2)Se_(3) solar cell and other optoelectronic devices.
基金supported by the National Natural Science Foundation of China(22275180)the National Key Research and Development Program of China(2019YFA0405600)the Collaborative Innovation Program of Hefei Science Center,CAS,and the University Synergy Innovation Program of Anhui Province(GXXT-2023-031).
文摘Cadmium sulfide(CdS)is an n-type semiconductor with excellent electrical conductivity that is widely used as an electron transport material(ETM)in solar cells.At present,numerous methods for preparing CdS thin films have emerged,among which magnetron sputtering(MS)is one of the most commonly used vacuum techniques.For this type of technique,the substrate temperature is one of the key deposition parameters that affects the interfacial properties between the target film and substrate,determining the specific growth habits of the films.Herein,the effect of substrate temperature on the microstructure and electrical properties of magnetron-sputtered CdS(MS-CdS)films was studied and applied for the first time in hydrothermally deposited antimony selenosulfide(Sb_(2)(S,Se)_(3))solar cells.Adjusting the substrate temperature not only results in the design of the flat and dense film with enhanced crystallinity but also leads to the formation of an energy level arrangement with a Sb_(2)(S,Se)_(3)layer that is more favorable for electron transfer.In addition,we developed an oxygen plasma treatment for CdS,reducing the parasitic absorption of the device and resulting in an increase in the short-circuit current density of the solar cell.This study demonstrates the feasibility of MS-CdS in the fabrication of hydrothermal Sb_(2)(S,Se)_(3)solar cells and provides interface optimization strategies to improve device performance.
基金financially supported by the National Natural Science Foundation of China(21003021 and 21373051)
文摘For a long time, there has been global concern over the environment and energy problems. Recently, the problems, which have brought about serious effect on the global living condition, have been in the ‘‘spotlight" and given impetus to the universal's efforts to head for the same direction: stem the worst warming and strive for the renewable energy source. Hydrogen peroxide(H_2O_2) is undoubtedly a good choice,which holds the promise as a clean, efficient, safe and transferrable energy carrier. Octahedral coordination polymer, Cd_3(C_3N_3S_3)_2, was found to be a robust photocatalyst for H_2O_2 generation under visible light irradiation. To further improve the H_2O_2 generation efficiency, adhering the octahedron to reduced graphene(rGO) was applied as the strategy herein. The study shows that by adhering Cd_3(C_3N_3S_3)_2to rGO, the formation of H_2O_2 is 2.5-fold enhanced and its deformation is concurrently suppressed. This work not only demonstrates the effectiveness of adhering Cd_3(C_3N_3S_3)_2polymer to rGO for the improvement of the polymer's photocatalytic performance, but also proposes a general way for the fabrication of graphene/coordination compound hybrids for maximizing their synergy.
基金partially supported by the National Natural Science Foundation of China(No.51672099 and 52073263)the Open Foundation of State Key Laboratory of Electronic Thin Films and Integrated Devices(No.KFJJ202105)Fundamental Research Funds for the Central Universities(No.2017-QR-25)。
文摘The production of renewable fossil fuels such as CH_(4) and CO by photocatalytic CO_(2)reduction has attracted more and more attention.However,single photocatalyst is less efficient for photocatalytic reduction of CO_(2)due to the fast recombination of photogenerated electron pairs.Herein,we successfully prepare CdS-Ag_(2)S composite by assembling the Ag_(2)S QDs cocatalyst on the surface of CdS nanosheet-assembled flower through oil-bath solvothermal method.This composite is prepared through a simple self-assembly strategy using cadmium chloride,ammonia and thiourea as precursors of the CdS nanosheet-assembled flower and silver nitrate and 3-mercaptopropionic acid as the precursors of Ag_(2)S QDs.The average diameter of Ag_(2)S QDs is apparently 6.0 nm.The light absorption edge of the composite is at around 560 nm,with the corresponding band gap at 2.14 eV.The CdS-Ag_(2)S QDs composite with 5 wt%Ag_(2)S QDs loaded achieves CO evolution rate of 16.6μmol·g^(-1)·h^(-1)without noble-metal cocatalysts.This strengthened photocatalytic performance and photocatalytic stability were attributed to the energy band broadening of Ag_(2)S QDs caused by quantum size effect and the large specific surface area due to the assembled flower.The mechanism underlying the enhanced photocatalytic CO_(2)reduction activity is further proposed.This study demonstrates that semiconductor-based quantum dots are strong candidates for excellent cocatalysts in photocatalysis.
基金the National Research Foundation of Korea(SRC-2017R1A5A1014560). This work was supported by grants from the National Research Foundation of Korea(SRC-2017R1A5A1014560)。
文摘Recombinant interleukin-33(IL-33)inhibits tumor growth,but the detailed immunological mechanism is still unknown.IL-33-mediated tumor suppression did not occur in Batf3^(−/−)mice,indicating that conventional type 1 dendritic cells(cDC1s)play a key role in IL-33-mediated antitumor immunity.A population of CD103^(+)cDC1s,which were barely detectable in the spleens of normal mice,increased significantly in the spleens of IL-33-treated mice.The newly emerged splenic CD103^(+)cDC1s were distinct from conventional splenic cDC1s based on their spleen residency,robust effector T-cell priming ability,and surface expression of FCGR3.DCs and DC precursors did not express Suppressor of Tumorigenicity 2(ST2).However,recombinant IL-33 induced spleen-resident FCGR3^(+)CD103^(+)cDC1s,which were found to be differentiated from DC precursors by bystander ST2+immune cells.Through immune cell fractionation and depletion assays,we found that IL-33-primed ST2^(+)basophils play a crucial role in the development of FCGR3^(+)CD103^(+)cDC1s by secreting IL-33-driven extrinsic factors.Recombinant GM-CSF also induced the population of CD103^(+)cDC1s,but the population neither expressed FCGR3 nor induced any discernable antitumor immunity.The population of FCGR3^(+)CD103^(+)cDC1s was also generated in vitro culture of Flt3L-mediated bone marrow-derived DCs(FL-BMDCs)when IL-33 was added in a pre-DC stage of culture.FL-BMDCs generated in the presence of IL-33(FL-33-DCs)offered more potent tumor immunotherapy than control Flt3L-BMDCs(FL-DCs).Human monocyte-derived DCs were also more immunogenic when exposed to IL-33-induced factors.Our findings suggest that recombinant IL-33 or an IL-33-mediated DC vaccine could be an attractive protocol for better tumor immunotherapy.
基金supported by the National Natural Science Foundation of China(No.21771061)Outstanding Youth Fund of Heilongjiang Province(No.JQ 2020B002).
文摘Designing photocatalysts with high light utilization and efficient photogenerated carrier separation for pollutant degradation is one of the important topics for sustainable development.In this study,hierarchical core–shell materialα-Fe_(2)O_(3)@ZnIn_(2)S_(4)with a step-scheme(S-scheme)heterojunction is synthesized by in situ growth technique,and MXene Ti_(3)C_(2)quantum dots(QDs)are introduced to construct a double-heterojunction tandem mechanism.The photodegradation efficiency ofα-Fe_(2)O_(3)@ZnIn_(2)S_(4)/Ti_(3)C_(2)QDs to bisphenol A is 96.1%and its reaction rate constant attained 0.02595 min^(−1),which is 12.3 times that of pureα-Fe_(2)O_(3).Meanwhile,a series of characterizations analyze the reasons for the enhanced photocatalytic activity,and the charge transport path of the S-scheme heterojunction/Schottky junction tandem is investigated.The construction of the S-scheme heterojunction enables the photo-generated electrons ofα-Fe_(2)O_(3)and the holes of ZnIn2S4 to transfer and combine under the action of the reverse built-in electric field.Due to the metallic conductivity of Ti_(3)C_(2)QDs,the photogenerated electrons of ZnIn_(2)S_(4)are further transferred to Ti_(3)C_(2)QDs to form a Schottky junction,which in turn forms a double-heterojunction tandem mechanism,showing a remarkable charge separation efficiency.This work provides a new opinion for the construction of tandem double heterojunctions to degrade harmful pollutants.
