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
Hydrothermal deposition of antimony selenosulfide(Sb_(2)(S,Se_(3)))has enabled solar cell applications to surpass the 10%efficiency threshold.This deposition process involves the reaction of three precursor materials:...Hydrothermal deposition of antimony selenosulfide(Sb_(2)(S,Se_(3)))has enabled solar cell applications to surpass the 10%efficiency threshold.This deposition process involves the reaction of three precursor materials:Sb,S,and Se.However,this process generates an unfavourable gradient of Se and S anions in the Sb_(2)(S,Se)_(3)film,which limits further efficiency improvements.Herein,we demonstrate how NH_(4)F can be used as an additive to regulate the band gradient of the Sb_(2)(S,Se)_(3)and modify the surface of the CdS electron-transporting layer.On the one hand,NH_(4)F inhibits the decomposition of Na_(2)S_(2)O_(3)and selenourea,which optimizes the deposition process and allows for adjustment of the Se/S ratio and their distribution in the Sb_(2)(S,Se)_(3)film.On the other hand,hydrolysis of NH_(4)F induces dissolution and redeposition of CdS,thereby effectively improving the morphology and crystallinity of the CdS substrate.Finally,the dual effect of NH_(4)F enables improved surface morphology and energy alignment of the Sb_(2)(S,Se)_(3)film,thus yielding a maximum efficiency of 10.28%,a 12%improvement over the control device.This study demonstrates an effective strategy for simultaneously modifying a sulfide-based substrate and regulating the element distribution during the deposition of a metal chalcogenide film for optoelectronic device applications.展开更多
High-throughput(HTP)experiments play key roles in accelerating the discovery of advanced materials,but the HTP preparation and characterization,especially for bulk samples,are extremely difficult.In this work,we devel...High-throughput(HTP)experiments play key roles in accelerating the discovery of advanced materials,but the HTP preparation and characterization,especially for bulk samples,are extremely difficult.In this work,we developed a novel and general strategy for HTP screening of high-performance bulk thermoelectric materials.The performed fullchain HTP experiments cover rapid synthesis of the bulk sample with quasi-continuous composition,microarea phase identification and structure analysis,and measurement of the spatial distribution of the sample composition,electrical and thermal transport properties.According to our experiments,bulk Bi_(2-x)Sb_(x)Te_(3)(x=1-2)and Bi_(2)Te_(3-x)Se_(x)(x=0-1.5)samples with quasi-continuous compositions have been rapidly fabricated by this HTP method.The target thermoelectric materials with the best Sb/Bi and Te/Se ratios are successfully screened out based on subsequent HTP characterization results,demonstrating that this HTP technique is effective in speeding up the exploration of novel high-performance thermoelectric materials.展开更多
Antimony chalcogenide Sb_(2)(S, Se)_(3) is attracting a lot of attention as photovoltaic absorber owing to its rewarding photoelectric properties, low toxicity, and earth abundance. However, its device efficiency is s...Antimony chalcogenide Sb_(2)(S, Se)_(3) is attracting a lot of attention as photovoltaic absorber owing to its rewarding photoelectric properties, low toxicity, and earth abundance. However, its device efficiency is still limited by the absorber material quality and device interface recombination. In this work, a fluorinedoped tin oxide(FTO) substrate with ultra-thin SnO_(2) layer and a low-cost stabilized carbon paste are introduced as a front and back contact layer respectively in Sb_(2)(S, Se)_(3) based planar solar cells. Over 5.2% efficiency is demonstrated in the structure of FTO/SnO_(2)/Cd S/Sb_(2)(S, Se)_3/Carbon/Ag, where the Sb_(2)(S, Se)_(3) is prepared by hydrothermal technique. The complementary device physics characterizations reveal that the interfacial recombination between TCO and Cd S is significantly suppressed by the introduction of ultra-thin SnO_(2) layer, which is profited from the leakage protection and bandgap offset engineering by its high resistivity and suitable conduction band minimum. Meanwhile, the successful adoption of the lowcost stabilized carbon as a back contact here shows an enormous potential to replace the conventional organic hole transport materials and noble metal. We hope this work can provide positive guidance to optimize Sb_(2)(S, Se)_(3) based planar solar cells in the future.展开更多
The use of organic hole transport layer(HTL)Spiro-OMeTAD in various solar cells imposes serious stabil-ity and cost problems,and thus calls for inorganic substitute materials.In this work,a novel inorganic MnS film pr...The use of organic hole transport layer(HTL)Spiro-OMeTAD in various solar cells imposes serious stabil-ity and cost problems,and thus calls for inorganic substitute materials.In this work,a novel inorganic MnS film prepared by thermal evaporation has been demonstrated to serve as a decent HTL in high-performance Sb_(2)(S,Se)_(3)solar cells,providing a cost-effective all-inorganic solution.A low-temperature air-annealing process for the evaporated MnS layer was found to result in a significant positive effect on the power conversion efficiency(PCE)of Sb_(2)(S,Se)_(3)solar cells,due to its better-matched energy band alignment after partial oxidation.Impressively,the device with the optimized MnS HTL has achieved an excellent PCE of about 9.24%,which is the highest efficiency among all-inorganic Sb_(2)(S,Se)_(3)solar cells.Our result has revealed that MnS is a feasible substitute for organic HTL in Sb-based solar cells to achieve high PCE,low cost,and high stability.展开更多
通过研究组分、掺杂和晶体生长条件对材料温差电性能的影响,采用熔炼—区熔法研制出较均匀的高性能赝三元 p 型温差电材料 Te:(Sb_2Te_3)_0.75(1-x)(Bi_2Te_3)_(0.25(1-x))(Sb_2Se_3)(?)生长出的晶锭的85%的部分,温差电优值 z=2.9~3.3&...通过研究组分、掺杂和晶体生长条件对材料温差电性能的影响,采用熔炼—区熔法研制出较均匀的高性能赝三元 p 型温差电材料 Te:(Sb_2Te_3)_0.75(1-x)(Bi_2Te_3)_(0.25(1-x))(Sb_2Se_3)(?)生长出的晶锭的85%的部分,温差电优值 z=2.9~3.3×10^(-3)/K。其性能高于目前国内的赝二元材料,达到了国外的较高水平,用这种材料制作的温差电致冷器件获得了很好的致冷效果。展开更多
Emulation of advanced synaptic functions of the human brain with electronic devices contributes an important step toward constructing high‐efficiency neuromorphic systems.Ferroelectric materials are promising candida...Emulation of advanced synaptic functions of the human brain with electronic devices contributes an important step toward constructing high‐efficiency neuromorphic systems.Ferroelectric materials are promising candidates as synaptic weight elements in neural network hardware due to their controllable polarization states.However,the increased depolarization field at the na-noscale and the complex fabrication process of the traditional ferroelectric materials hamper the development of high‐density,low‐power,and highly sensitive synaptic devices.Here,we report the implementation of two‐dimensional(2D)ferroelectricα‐In_(2)Se_(3)as an active channel material to emulate typical synaptic functions.Theα‐In_(2)Se_(3)‐based synaptic device fea-tures multimode operations,enabled by the coupled ferroelectric polarization under various voltage pulses applied at both drain and gate terminals.Moreover,the energy consumption can be reduced to~1 pJ by using high‐κdielectric(Al2O3).The successful control of ferroelectric polarizations inα‐In_(2)Se_(3)and its application in artificial synapses are expected to inspire the implementation of 2D ferroelectric materials for future neuromorphic systems.展开更多
Antimony selenide(Sb_(2)Se_(3))is a promising candidate for photodetector applications boasting unique material benefits and remarkable optoelectronic properties.Achieving high-performance self-powered Sb_(2)Se_(3)pho...Antimony selenide(Sb_(2)Se_(3))is a promising candidate for photodetector applications boasting unique material benefits and remarkable optoelectronic properties.Achieving high-performance self-powered Sb_(2)Se_(3)photodetector through a synergistic regulation of absorber layer and heterojunction interface demonstrates great potential and needs essential investigation.In this study,an effective two-step thermodynamic/kinetic deposition technique containing sputtered and selenized Sb precursor is implemented to induce self-assembled growth of Sb_(2)Se_(3)light absorbing thin film with large crystal grains and desirable[hk1]orientation,presenting considerable thin-film photodetector performance.Furthermore,aluminum(Al^(3+))cation dopant is introduced to modify the optoelectronic properties of CdS buffer layer,and further optimize the Sb_(2)Se_(3)/CdS(Al)heterojunction interface quality.Thanks to the suppressed carrier recombination and enhanced carrier transport kinetics,the champion Mo/Sb_(2)Se_(3)/CdS(Al)/ITO/Ag photodetector exhibits self-powered and broadband characteristics,accompanied by simultaneously high responsivity of 0.9 A W^(-1)(at 11 nW cm^(-2)),linear dynamic range of 120 dB,impressive ON/OFF switching ratio over 10^(6)and signal-to-noise ratio of 10^(9),record total noise determined realistic detectivity of 4.78×10^(12)Jones,and ultra-fast response speed with rise/decay time of 24/75 ns,representing the top level for Sb_(2)Se_(3)-based photodetectors.This intriguing work opens up an avenue for its selfpowered broadband photodetector applications.展开更多
基于像差校正扫描透射电子显微学和第一性原理计算,研究了van der Waals(范德瓦尔斯)层状β-In_(2)Se_(3)中堆垛缺陷的原子构型。结果表明,在2Hβ-In_(2)Se_(3)中存在大量的置换型层错(RSF)和滑移型层错(SSF),发现了一种在热力学上易自...基于像差校正扫描透射电子显微学和第一性原理计算,研究了van der Waals(范德瓦尔斯)层状β-In_(2)Se_(3)中堆垛缺陷的原子构型。结果表明,在2Hβ-In_(2)Se_(3)中存在大量的置换型层错(RSF)和滑移型层错(SSF),发现了一种在热力学上易自发形成的T相滑移型堆垛层错(tSSF);在3Rβ-In_(2)Se_(3)中只观察到一种能量较高的滑移型层错;2H和3Rβ-In_(2)Se_(3)以界面连续过渡的方式发生相分离。本文还构建9种β-In_(2)Se_(3)潜在的堆垛层错构型,并计算了相应的堆垛层错能并从能量角度分析了堆垛层错的成因。最后,指出建立分类术语描述类van der Waals层状材料堆垛层错的必要性。展开更多
It is a challenging issue to further drive charge separation through the oriented design of Z-scheme het-erojunction in the exploitation of cost-effective photocatalytic materials.In this contribution,the unique Z-sch...It is a challenging issue to further drive charge separation through the oriented design of Z-scheme het-erojunction in the exploitation of cost-effective photocatalytic materials.In this contribution,the unique Z-scheme 3D/2D In_(2)Se_(3)/PCN heterojunction is developed through implanting In_(2)Se_(3) microspheres on PCN nanosheets using an in situ growth technique,which acquires the effective CO generation activity from photocatalytic CO_(2) reduction(CO_(2)R).The CO yield of 4 h in the CO_(2)R reaction over the optimal In_(2)Se_(3)/PCN-15 sample reaches up to 11.40 and 2.41 times higher than that of individual PCN and In_(2)Se_(3),respectively.Such greatly enhanced photocatalytic performance is primarily the improvement of photo-generated carrier separation efficiency.To be more specific,the formed built-in electric field is signifi-cantly intensified by producing the temperature difference potential between In_(2)Se_(3) and PCN owing to the photothermoelectric effect of In_(2)Se_(3),which actuates the high-efficiency separation of photogenerated charge carriers along the Z-scheme transfer path in the In_(2)Se_(3)/PCN heterojunction.The effective strat-egy of enhancing the built-in electric field to drive photogenerated charge separation proposed in this work opens up an innovative avenue to design Z-scheme heterojunction applied to high-efficiency pho-tocatalytic reactions,such as hydrogen generation from water splitting,CO_(2)R,and degradation of organic pollutants.展开更多
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the National Natural Science Foundation of China(22005293 and U19A2092)the National Key Research and Development Program of China(2019YFA0405600).
文摘Hydrothermal deposition of antimony selenosulfide(Sb_(2)(S,Se_(3)))has enabled solar cell applications to surpass the 10%efficiency threshold.This deposition process involves the reaction of three precursor materials:Sb,S,and Se.However,this process generates an unfavourable gradient of Se and S anions in the Sb_(2)(S,Se)_(3)film,which limits further efficiency improvements.Herein,we demonstrate how NH_(4)F can be used as an additive to regulate the band gradient of the Sb_(2)(S,Se)_(3)and modify the surface of the CdS electron-transporting layer.On the one hand,NH_(4)F inhibits the decomposition of Na_(2)S_(2)O_(3)and selenourea,which optimizes the deposition process and allows for adjustment of the Se/S ratio and their distribution in the Sb_(2)(S,Se)_(3)film.On the other hand,hydrolysis of NH_(4)F induces dissolution and redeposition of CdS,thereby effectively improving the morphology and crystallinity of the CdS substrate.Finally,the dual effect of NH_(4)F enables improved surface morphology and energy alignment of the Sb_(2)(S,Se)_(3)film,thus yielding a maximum efficiency of 10.28%,a 12%improvement over the control device.This study demonstrates an effective strategy for simultaneously modifying a sulfide-based substrate and regulating the element distribution during the deposition of a metal chalcogenide film for optoelectronic device applications.
基金supported by the National Key Research and Development Program of China(2018YFB0703600 and 2018YFA0702100)the National Natural Science Foundation of China(51772186,51632005 and 51371194)。
文摘High-throughput(HTP)experiments play key roles in accelerating the discovery of advanced materials,but the HTP preparation and characterization,especially for bulk samples,are extremely difficult.In this work,we developed a novel and general strategy for HTP screening of high-performance bulk thermoelectric materials.The performed fullchain HTP experiments cover rapid synthesis of the bulk sample with quasi-continuous composition,microarea phase identification and structure analysis,and measurement of the spatial distribution of the sample composition,electrical and thermal transport properties.According to our experiments,bulk Bi_(2-x)Sb_(x)Te_(3)(x=1-2)and Bi_(2)Te_(3-x)Se_(x)(x=0-1.5)samples with quasi-continuous compositions have been rapidly fabricated by this HTP method.The target thermoelectric materials with the best Sb/Bi and Te/Se ratios are successfully screened out based on subsequent HTP characterization results,demonstrating that this HTP technique is effective in speeding up the exploration of novel high-performance thermoelectric materials.
基金supported by the National Natural Science Foundation of China (22005293, U19A2092 and 22275180)the National Key Research and Development Program of China (2019YFA0405600)+1 种基金the Institute of Energy, Hefei Comprehensive National Science Center (21KZS212)the Collaborative Innovation Program of Hefei Science Center, CAS。
基金supported by National Natural Science Foundation of China (Grant No. 61974028)Fujian Normal University(FNU) Training Program of Innovation and Enterpreneurship for Undergraduates (cxxl-2019135+2 种基金20191402019143)the support from Huai An Yaoke Optoelectronics Co.Ltd。
文摘Antimony chalcogenide Sb_(2)(S, Se)_(3) is attracting a lot of attention as photovoltaic absorber owing to its rewarding photoelectric properties, low toxicity, and earth abundance. However, its device efficiency is still limited by the absorber material quality and device interface recombination. In this work, a fluorinedoped tin oxide(FTO) substrate with ultra-thin SnO_(2) layer and a low-cost stabilized carbon paste are introduced as a front and back contact layer respectively in Sb_(2)(S, Se)_(3) based planar solar cells. Over 5.2% efficiency is demonstrated in the structure of FTO/SnO_(2)/Cd S/Sb_(2)(S, Se)_3/Carbon/Ag, where the Sb_(2)(S, Se)_(3) is prepared by hydrothermal technique. The complementary device physics characterizations reveal that the interfacial recombination between TCO and Cd S is significantly suppressed by the introduction of ultra-thin SnO_(2) layer, which is profited from the leakage protection and bandgap offset engineering by its high resistivity and suitable conduction band minimum. Meanwhile, the successful adoption of the lowcost stabilized carbon as a back contact here shows an enormous potential to replace the conventional organic hole transport materials and noble metal. We hope this work can provide positive guidance to optimize Sb_(2)(S, Se)_(3) based planar solar cells in the future.
基金the Science and Technology Department of Hubei Province(2019AAA020)Wuhan Science and Technology Project of China(2019010701011420)+1 种基金Fundamental Research Funds for the Central University(2042021kf0069)the National Natural Science Foundation of China(61974028)。
文摘The use of organic hole transport layer(HTL)Spiro-OMeTAD in various solar cells imposes serious stabil-ity and cost problems,and thus calls for inorganic substitute materials.In this work,a novel inorganic MnS film prepared by thermal evaporation has been demonstrated to serve as a decent HTL in high-performance Sb_(2)(S,Se)_(3)solar cells,providing a cost-effective all-inorganic solution.A low-temperature air-annealing process for the evaporated MnS layer was found to result in a significant positive effect on the power conversion efficiency(PCE)of Sb_(2)(S,Se)_(3)solar cells,due to its better-matched energy band alignment after partial oxidation.Impressively,the device with the optimized MnS HTL has achieved an excellent PCE of about 9.24%,which is the highest efficiency among all-inorganic Sb_(2)(S,Se)_(3)solar cells.Our result has revealed that MnS is a feasible substitute for organic HTL in Sb-based solar cells to achieve high PCE,low cost,and high stability.
文摘通过研究组分、掺杂和晶体生长条件对材料温差电性能的影响,采用熔炼—区熔法研制出较均匀的高性能赝三元 p 型温差电材料 Te:(Sb_2Te_3)_0.75(1-x)(Bi_2Te_3)_(0.25(1-x))(Sb_2Se_3)(?)生长出的晶锭的85%的部分,温差电优值 z=2.9~3.3×10^(-3)/K。其性能高于目前国内的赝二元材料,达到了国外的较高水平,用这种材料制作的温差电致冷器件获得了很好的致冷效果。
基金Ministry of Education—Singapore,Grant/Award Number:MOE‐2019‐T2‐1‐002National Natural Science Foundation of China,Grant/Award Numbers:21872100,U2032147Agency for Science,Technology and Research,Grant/Award Numbers:A1938c0035,A20G9b0135。
文摘Emulation of advanced synaptic functions of the human brain with electronic devices contributes an important step toward constructing high‐efficiency neuromorphic systems.Ferroelectric materials are promising candidates as synaptic weight elements in neural network hardware due to their controllable polarization states.However,the increased depolarization field at the na-noscale and the complex fabrication process of the traditional ferroelectric materials hamper the development of high‐density,low‐power,and highly sensitive synaptic devices.Here,we report the implementation of two‐dimensional(2D)ferroelectricα‐In_(2)Se_(3)as an active channel material to emulate typical synaptic functions.Theα‐In_(2)Se_(3)‐based synaptic device fea-tures multimode operations,enabled by the coupled ferroelectric polarization under various voltage pulses applied at both drain and gate terminals.Moreover,the energy consumption can be reduced to~1 pJ by using high‐κdielectric(Al2O3).The successful control of ferroelectric polarizations inα‐In_(2)Se_(3)and its application in artificial synapses are expected to inspire the implementation of 2D ferroelectric materials for future neuromorphic systems.
基金supported by National Natural Science Foundation of China(No.62104156,62074102)Guangdong Basic and Applied Basic Research Foundation(2020A1515010805,2022A1515010979)China+1 种基金Science and Technology plan project of Shenzhen(20200812000347001,20220808165025003)Chinasupported by open foundation of Guangxi Key Laboratory of Processing for Non-ferrous Metals and Featured Materials,Guangxi University(Grant No.2022GXYSOF13)。
文摘Antimony selenide(Sb_(2)Se_(3))is a promising candidate for photodetector applications boasting unique material benefits and remarkable optoelectronic properties.Achieving high-performance self-powered Sb_(2)Se_(3)photodetector through a synergistic regulation of absorber layer and heterojunction interface demonstrates great potential and needs essential investigation.In this study,an effective two-step thermodynamic/kinetic deposition technique containing sputtered and selenized Sb precursor is implemented to induce self-assembled growth of Sb_(2)Se_(3)light absorbing thin film with large crystal grains and desirable[hk1]orientation,presenting considerable thin-film photodetector performance.Furthermore,aluminum(Al^(3+))cation dopant is introduced to modify the optoelectronic properties of CdS buffer layer,and further optimize the Sb_(2)Se_(3)/CdS(Al)heterojunction interface quality.Thanks to the suppressed carrier recombination and enhanced carrier transport kinetics,the champion Mo/Sb_(2)Se_(3)/CdS(Al)/ITO/Ag photodetector exhibits self-powered and broadband characteristics,accompanied by simultaneously high responsivity of 0.9 A W^(-1)(at 11 nW cm^(-2)),linear dynamic range of 120 dB,impressive ON/OFF switching ratio over 10^(6)and signal-to-noise ratio of 10^(9),record total noise determined realistic detectivity of 4.78×10^(12)Jones,and ultra-fast response speed with rise/decay time of 24/75 ns,representing the top level for Sb_(2)Se_(3)-based photodetectors.This intriguing work opens up an avenue for its selfpowered broadband photodetector applications.
文摘基于像差校正扫描透射电子显微学和第一性原理计算,研究了van der Waals(范德瓦尔斯)层状β-In_(2)Se_(3)中堆垛缺陷的原子构型。结果表明,在2Hβ-In_(2)Se_(3)中存在大量的置换型层错(RSF)和滑移型层错(SSF),发现了一种在热力学上易自发形成的T相滑移型堆垛层错(tSSF);在3Rβ-In_(2)Se_(3)中只观察到一种能量较高的滑移型层错;2H和3Rβ-In_(2)Se_(3)以界面连续过渡的方式发生相分离。本文还构建9种β-In_(2)Se_(3)潜在的堆垛层错构型,并计算了相应的堆垛层错能并从能量角度分析了堆垛层错的成因。最后,指出建立分类术语描述类van der Waals层状材料堆垛层错的必要性。
基金National Natural Science Foundation of China(Nos.52072153 and 62004143)Key R&D Program of Hubei Province(No.2022BAA084)+2 种基金Postdoctoral Science Foundation of China(No.2021M690023)Graduate Research Innovation Program of Jiangsu Provincial(Nos.KYCX22_3694 and KYCX23_3649)Zhenjiang Key R&D Programmes(No.SH2021021).
文摘It is a challenging issue to further drive charge separation through the oriented design of Z-scheme het-erojunction in the exploitation of cost-effective photocatalytic materials.In this contribution,the unique Z-scheme 3D/2D In_(2)Se_(3)/PCN heterojunction is developed through implanting In_(2)Se_(3) microspheres on PCN nanosheets using an in situ growth technique,which acquires the effective CO generation activity from photocatalytic CO_(2) reduction(CO_(2)R).The CO yield of 4 h in the CO_(2)R reaction over the optimal In_(2)Se_(3)/PCN-15 sample reaches up to 11.40 and 2.41 times higher than that of individual PCN and In_(2)Se_(3),respectively.Such greatly enhanced photocatalytic performance is primarily the improvement of photo-generated carrier separation efficiency.To be more specific,the formed built-in electric field is signifi-cantly intensified by producing the temperature difference potential between In_(2)Se_(3) and PCN owing to the photothermoelectric effect of In_(2)Se_(3),which actuates the high-efficiency separation of photogenerated charge carriers along the Z-scheme transfer path in the In_(2)Se_(3)/PCN heterojunction.The effective strat-egy of enhancing the built-in electric field to drive photogenerated charge separation proposed in this work opens up an innovative avenue to design Z-scheme heterojunction applied to high-efficiency pho-tocatalytic reactions,such as hydrogen generation from water splitting,CO_(2)R,and degradation of organic pollutants.