Owing to their unique physicochemical,optical and electrical properties,two-dimensional(2D)MoS_(2) cocatalysts have been widely applied in designing and developing highly efficient composite photocatalysts for hydroge...Owing to their unique physicochemical,optical and electrical properties,two-dimensional(2D)MoS_(2) cocatalysts have been widely applied in designing and developing highly efficient composite photocatalysts for hydrogen generation under suitable light irradiation.In this review,we first elaborated on the fundamental aspects of 2D MoS_(2) cocatalysts to include the structural design principles,synthesis strategies,strengths and challenges.Subsequently,we thoroughly highlighted and discussed the modification strategies of 2D MoS_(2) H2-evolution cocatalysts,including doping heteroatoms(e.g.metals,non-metals,and co-doping),designing interfacial coupling morphologies,controlling the physical properties(e.g.thickness,size,structural defects or pores),exposing the reactive facets or edge sites,constructing cocatalyst heterojunctions,engineering the interfacial bonds and confinement effects.In the future,the forefront challenges in understanding and in precise controlling of the active sites at molecular level or atomic level should be carefully studied,while various potential mechanisms of photogenerated-electrons interactions should be proposed.The applications of MoS_(2) cocatalyst in the overall water splitting are also expected.This review may offer new inspiration for designing and constructing novel and efficient MoS_(2)-based composite photocatalysts for highly efficient photocatalytic hydrogen evolution.展开更多
Rational design and controllable synthesis of efficient electrocatalysts for water oxidation is of significant importance for the development of promising energy conversion systems, in particular integrated photoelect...Rational design and controllable synthesis of efficient electrocatalysts for water oxidation is of significant importance for the development of promising energy conversion systems, in particular integrated photoelectrochemical water splitting devices. Cobalt oxide(Co3O4) nanostructures with mixed valences(Ⅱ,Ⅲ)have been regarded as promising electrocatalysts for the oxygen evolution reaction(OER). They are able to promote catalytic support of OER but with only modest activity. Here, we demonstrate that the OER performance of cubic Co3O4 electrocatalyst is obviously improved when they are anchored on delaminated two-dimensional(2D) Ti3C2 MXene nanosheets. Upon activation the overpotential of the hybrid catalyst delivers 300 m V at a current density of 10 m A cm(2) in basic solutions, which is remarkably lower than those of Ti3C2 MXene and Co3O4 nanocubes. The strong interfacial electrostatic interactions between two components contribute to the exceptional catalytic performance and stability. The enhanced OER activity and facile synthesis make these Co3O4 nanocubes-decorated ultrathin 2D Ti3C2 MXene nanosheets useful for constructing efficient and stable electrodes for high-performance electrochemical water splitting.展开更多
Photoelectrochemical(PEC)water splitting is recognized as a sustainable strategy for hydrogen generation due to its abundant hydrogen source,utilization of inexhaustible solar energy,high-purity product,and environmen...Photoelectrochemical(PEC)water splitting is recognized as a sustainable strategy for hydrogen generation due to its abundant hydrogen source,utilization of inexhaustible solar energy,high-purity product,and environment-friendly process.To actualize a practical PEC water splitting,it is paramount to develop efficient,stable,safe,and low-cost photoelectrode materials.Recently,graphitic carbon nitride(g-C3N4)has aroused a great interest in the new generation photoelectrode materials because of its unique features,such as suitable band structure for water splitting,a certain range of visible light absorption,nontoxicity,and good stability.Some inherent defects of g-C3N4,however,seriously impair further improvement on PEC performance,including low electronic conductivity,high recombination rate of photogenerated charges,and limited visible light absorption at long wavelength range.Construction of g-C3N4-based nanosized heteroarrays as photoelectrodes has been regarded as a promising strategy to circumvent these inherent limitations and achieve the high-performance PEC water splitting due to the accelerated exciton separation and the reduced combination of photogenerated electrons/holes.Herein,we summarize in detail the latest progress of g-C3N4-based nanosized heteroarrays in PEC water-splitting photoelectrodes.Firstly,the unique advantages of this type of photoelectrodes,including the highly ordered nanoarray architectures and the heterojunctions,are highlighted.Then,different g-C3N4-based nanosized heteroarrays are comprehensively discussed,in terms of their fabrication methods,PEC capacities,and mechanisms,etc.To conclude,the key challenges and possible solutions for future development on g-C3N4-based nanosized heteroarray photoelectrodes are discussed.展开更多
In this study, CdS/g-C3N4 （CSCN） heterojunctions were in situ fabricated with a large amount of CdS nanoparticles anchored on g-C3N4 nanosheets, A wet chemical method was developed for the first time to determine th...In this study, CdS/g-C3N4 （CSCN） heterojunctions were in situ fabricated with a large amount of CdS nanoparticles anchored on g-C3N4 nanosheets, A wet chemical method was developed for the first time to determine the actual content of CdS in CSCN composites. X-ray diffraction （XRD）, Fourier transform infrared spectra （FFIR）, high-resolution transmission electron microscopy （HRTEM） and UV-vis diffuse reflectance spectra （DRS） were employed to characterize the composition, structure and optical prop- erty of CSCN composites. Based on the is0electric point （liP） analysis of g-C3N4, a conclusion was obtained on the combination mechanism between CdS nanoparticles and g-C3N4 nanosheets. The photocatalytic activity of CSCN composites was much better than those of individual CdS and g-C3N4 for the degrada- tion of azo dye Methyl Orange （MO） by 40 min adsorption in the dark followed by 15 min photocatalysis under visible light irradiation. After 5 cycles, CSCN composites still maintained high reactive activity with the MO degradation efficiency of 93.8%, exhibiting good photocatalytic stability. The Cd2~ concentration dissolved in the supernatant detected by atomic absorption spectroscopy （AAS） of CSCN composites was lower than that of pure CdS, implying that the photocorrosion of CdS could be suppressed via the combination with g-C3N4. Photoluminescence emission spectra （PL） results clearly revealed that the recombination of photogenerated electron-hole pairs in CSCN composites was effectively inhibited due to the formation of heterojunctions. Based on the band alignments of g-C3N4 and CdS, the possible photocatalvtic mechnism was discussed.展开更多
As a choke point in water electrolysis,the oxygen evolution reaction(OER)suffers from the severe electrode polarization and large overpotential.Herein,the porous hierarchical hetero-(Nis Fe)FeN/Ni catalysts are in sit...As a choke point in water electrolysis,the oxygen evolution reaction(OER)suffers from the severe electrode polarization and large overpotential.Herein,the porous hierarchical hetero-(Nis Fe)FeN/Ni catalysts are in situ constructed for the eficient electrocatalytic OER.X-ray absorption fine structure characterizations reveal the strong Ni-Fe bimetallic interaction in(Niz Fex)FeN/Ni.Theoretical study indicates the heterojunction and bimetallic interaction decrease the free-energy change for the rate-limiting step of the OER and the overpotential thereof.In addition,the high conductivity and porous hierarchical morphology favor the electron transfer,electrolyte access and O2 release.Consequently,the optimized catalyst achieves a low overpotential of 223 mV at 10 mA.cm^-2,a small Tafel slope of 68 mV:dec^-1,and a high stability.The excellent performance of the optimized catalyst is also demonstrated by the overall water electrolysis with a low working voltage and high Faradaic efficiency.Moreover,the correlation between the structure and performance is well established by the experimental characterizations and theoretical calculations,which confirms the origin of the OER activity from the surface metal oxyhydroxide in situ generated upon applying the current.This study suggests a promising approach to the advanced OER electrocatalysts for practical applications by constructing the porous hierarchical metal-compound/metal heterojunctions.展开更多
As one of the most important semiconductor materials, silicon （Si） has been widely used in current energy and optoelectronic devices, such as solar cells and photodetectors. However, the traditional Si p-n junction ...As one of the most important semiconductor materials, silicon （Si） has been widely used in current energy and optoelectronic devices, such as solar cells and photodetectors. However, the traditional Si p-n junction solar cells need complicated fabrication processes, leading to the high cost of Si photovoltaic devices. The wide applications of Si-based photodetectors are also hampered by their low sensitivity to ultraviolet and infrared light. Recently, two-dimensional （2D） layered materials have emerged as a new material system with tremendous potential for future energy and optoelectronic applications. The combination of Si with 2D layered materials represents an innovative approach to construct high-performance optoelectronic devices by harnessing the complementary advantages of both materials. In this review, we summarize the recent advances in 2D layered material/Si heterojunctions and their applications in photovoltaic and optoelectronic devices. Finally, the outlook and challenges of 2D layered material/Si heterojunctions for high-performance device applications are presented.展开更多
Photocatalysis is believed to be one of the best methods to realize sustainable H2 production. However, achieving this through heterogeneous photocatalysis still remains a great challenge owing to the absence of activ...Photocatalysis is believed to be one of the best methods to realize sustainable H2 production. However, achieving this through heterogeneous photocatalysis still remains a great challenge owing to the absence of active sites, sluggish surface reaction kinetics, insufficient charge separation, and a high thermodynamic barrier. Therefore, cocatalysts are necessary and of great significance in boosting photocatalytic H2 generation. This review will focus on the promising and appealing low-cost Ni-based H2-generation cocatalysts as the alternatives for the high-cost and low-abundance noble metal cocatalysts. Special emphasis has been placed on the design principle, modification strategies for further enhancing the activity and stability of Ni-based cocatalysts, and identification of the exact active sites and surface reaction mechanisms. Particularly, four types of modification strategies based on increased light harvesting, enhanced charge separation, strengthened interface interaction, and improved electrocatalytic activity have been thoroughly discussed and compared in detail. This review may open a new avenue for designing highly active and durable Ni-based cocatalysts for photocatalytic H2 generation.展开更多
Novel SnO2-x/g-C3N4 heterojunction nanocomposites composed of reduced SnO2 nanoparticles and exfoliated g-CBN4 nanosheets were prepared by a convenient one-step pyrolysis method. The structural, morphological, and opt...Novel SnO2-x/g-C3N4 heterojunction nanocomposites composed of reduced SnO2 nanoparticles and exfoliated g-CBN4 nanosheets were prepared by a convenient one-step pyrolysis method. The structural, morphological, and optical properties of the as-prepared nanocomposites were characterized in detail, indicating that the aggregation of g-C3N4 nanosheets was prevented by small, well-dispersed SnO2_x nanoparticles. The ultraviolet-visible spectroscopy absorption bands of the nanocomposites were shifted to a longer wavelength region than those exhibited by pure SnO2 or g-CgN4. The charge transfer and recombination processes occurring in the nanocomposites were investigated using linear scan voltammetry and electrochemical impedance spectroscopy. Under 30-W visible-light-emitting diode irradiation, the heterojunction containing 27.4 wt.% SnO2-x exhibited the highest photocurrent density of 0.0468 mA.cm-2, which is 33.43 and 5.64 times larger than that of pure SnO2 and g-C3N4, respectively. The photocatalytic activity of the heterojunction material was investigated by degrading rhodamine B under irradiation from the same light source. Kinetic study revealed a promising degradation rate constant of 0.0226 min^-1 for the heterojunction containing 27.4 wt.% SnO2-x, which is 32.28 and 5.79 times higher than that of pure SnO2 and g-C3N4, respectively. The enhanced photoelectrochemical and photocatalytic performances of the nanocomposite may be due to its appropriate SnO2x content and the compact structure of the junction between the SnO2-x nanoparticles and the g-C3N4 nanosheets, which inhibits the recombination of photogenerated electrons and holes.展开更多
The formation of heterojunction within solid-state devices enables them with eventually high performances,but provides a challenge for material synthesis and device fabrication because strict conditions such as lattic...The formation of heterojunction within solid-state devices enables them with eventually high performances,but provides a challenge for material synthesis and device fabrication because strict conditions such as lattice match are needed.Herein,we show a facile method to fabricate a van der Waals(vdW)heterojunction between two-dimensional(2D)bismuth oxyselenide(Bi2O2Se)and graphene,during which the graphene is directly transferred to the Bi2O2Se and served as a lowcontract-resistant electrode with small work function mismatch(~50 meV).As an optoelectronic device,the Bi2O2Se/graphene vdW heterojunction allows for the efficient sensing toward 1200-nm incident laser.Regarding the application of fieldeffect transistors(FETs),the short-channel(50 nm)sample can be synthesized by utilizing these two 2D materials(ie,channel:Bi2O2Se;drain/source terminal:graphene)and the n-type characteristic can be observed with the accordant field modulation.It is confirmed that we show a simple way to prepare the vdW heterojunction which is aiming to the high-performance applications among optoelectronics and FETs.展开更多
The traditional single material with two-dimensional （2D） biomimetic moth-eye structures is limited by its narrowband antireflection and single functional capability. To overcome these disadvantages, we exploited we...The traditional single material with two-dimensional （2D） biomimetic moth-eye structures is limited by its narrowband antireflection and single functional capability. To overcome these disadvantages, we exploited wet etching and hydrothermal synthesis coupled with chemical oxidation for fabricating a three- dimensional （3D） biomimetic moth-eye coating with ternary materials （polypyrrole nanoparticles, TiO2 nanorods, and Si micropyramids, i.e., PPy/TiOa/Si-p）. This coating reduced the reflectivity to 〈4% at wavelengths ranging from 200 to 2,300 nm and exhibited remarkable superhydrophilidty with a low water contact angle of 1.8°. Moreover, the composite coating had double p-n heterojunctions, allowing the high-efficiency separation of photogenerated carriers. The photo- current density of PPy/TiO2/Si-p was more than three times higher than that of TiO2/Si-p at a positive potential of 1.5 V. The proposed method provides a means to enhance solar energy conversion.展开更多
Photoelectrochemical(PEC)technology is considered to be a promising approach for solar-driven hydrogen production with zero emissions.Bismuth vanadate(BiVO_(4))is a kind of photocatalytic material with strong photoact...Photoelectrochemical(PEC)technology is considered to be a promising approach for solar-driven hydrogen production with zero emissions.Bismuth vanadate(BiVO_(4))is a kind of photocatalytic material with strong photoactivity in the visible light region and appropriate band gap for PEC water splitting.However,the solar-to-hydrogen efficiency(STH)of BiVO_(4)is far away from the 10%target needed for practical application due to its poor charge separation ability.Therefore,this review attempts to summarize the strategies for improving the photocurrent density and especially hydrogen production of BiVO_(4)materials through PEC techniques in the last three years,such as doping nonmetal and metal elements,depositing noble metals,constructing heterojunctions,coupling with carbon and metalorganic framework(MOF)materials to further enhance the PEC performance of BiVO_(4)photoanode.This review aims to serve as a general guideline to fabricate highly efficient BiVO_(4)-based materials for PEC water splitting.展开更多
Carbon nitride-based photocatalysts hold an enormous potential in producing hydrogen.A strategy to simultaneously create isotype heterojunctions and active sites in highly-crystallized carbon nitride is anticipated to...Carbon nitride-based photocatalysts hold an enormous potential in producing hydrogen.A strategy to simultaneously create isotype heterojunctions and active sites in highly-crystallized carbon nitride is anticipated to significantly boost the photocatalytic activity,but is yet to be realized.Herein,we find that cobalt salt added in the ionothermal synthesis can promote the phase transition of heptazine-based crystalline carbon nitride(CCN)to triazine-based poly(triazine imide)(PTI),rendering the creation of singleatom cobalt coordinated isotype CCN/PTI heterojunction.Co-CCN/PTI exhibits an appreciable apparent quantum yield of 20.88%at 425 nm for photocatalytic hydrogen production with a rate achieving3538μmol h^(-1)g^(-1)(λ>420 nm),which is 4.8 times that of CCN and 27.6 times that of PTI.The high photocatalytic activity is attributed to the Type II isotype highly-crystallized CCN/PTI heterojunction for promoting charge carrier migration,and the single-atom Co sites for accelerating surface oxidation reaction.展开更多
Developing effective strategies to improve the initial Coulombic efficiency(ICE)and cycling stability of hard carbon(HC)anodes for sodium-ion batteries is the key to promoting the commercial application of HC.In this ...Developing effective strategies to improve the initial Coulombic efficiency(ICE)and cycling stability of hard carbon(HC)anodes for sodium-ion batteries is the key to promoting the commercial application of HC.In this paper,homotype heterojunctions are designed on HC to induce the generation of stable solid electrolyte interfaces,which can effectively increase the ICE of HC from 64.7%to 81.1%.The results show that using a simple surface engineering strategy to construct a homotypic amorphous Al_(2)O_(3) layer on the HC could shield the active sites,and further inhibit electrolyte decomposition and side effects occurrence.Particularly,due to the suppression of continuous decomposition of NaPF 6 in ester-based electrolytes,the accumulation of NaF could be reduced,leading to the formation of thinner and denser solid electrolyte interface films and a decrease in the interface resistance.The HC anode can not only improve the ICE but elevate its sodium storage performance based on this homotype heterojunction composed of HC and Al_(2)O_(3).The optimized HC anode exhibits an outstanding reversible capacity of 321.5mAhg^(−1) at 50mAg^(−1).The cycling stability is also improved effectively,and the capacity retention rate is 86.9%after 2000 cycles at 1Ag^(−1) while that of the untreated HC is only 52.6%.More importantly,the improved sodium storage behaviors are explained by electrochemical kinetic analysis.展开更多
Van der Waals （vdW） heterojunctions based on two-dimensional （2D） atomic crystals have been extensively studied in recent years. Herein, we show that both vertical and lateral vdW heterojunctions can be realized w...Van der Waals （vdW） heterojunctions based on two-dimensional （2D） atomic crystals have been extensively studied in recent years. Herein, we show that both vertical and lateral vdW heterojunctions can be realized with layered molecular crystals using a two-step physical vapor transport （PVT） process. Both types of heterojunctions show clean and sharp interfaces without phase mixing under atomic force microscopy （AFM）. They also exhibit a strong interfacial built-in electric field similar to that of their inorganic counterparts. These heterojunctions have greater potential for device applications than individual materials. The lateral heterojunction （LHJ） devices show rectifying characteristics due to the asymmetric energy barrier for holes at the interface, while the vertical heterojunction （VHJ） devices behave like metal-insulator-semiconductor tunnel junctions, with pronounced negative differential conductance （NDC）. Our work extends the concept of vdW heterojunctions to molecular materials, which can be generalized to other layered organic semiconductors （OSCs） to obtain new device functionalities.展开更多
A photonic heterostructure with multi-channel and sharp angular defect modes by combining two different one-dimensional defective photonic crystals is proposed. The filters designed on the basis of this heterostructur...A photonic heterostructure with multi-channel and sharp angular defect modes by combining two different one-dimensional defective photonic crystals is proposed. The filters designed on the basis of this heterostructure possess both functions of multi-channel narrow band filtering and sharp angular filtering. The channels, channel interval, and number of channels can be tuned by adjusting the geometric and physical parameters of the heterostuctures. This kind of filters will benefit the development of multi-channel interstellar or atmosphere optical communication.展开更多
基金the National Natural Science Foundation of China(Nos.21975084 and 51672089)the Guangdong Provincial Applied Science and Technology Research and Development Program(No.2017B020238005)+2 种基金the Ding Ying Talent Project of South China Agricultural University for their supportthe Hong Kong Research Grant Council(RGC)General Research Fund(No.GRF1305419)for financial supportthe National Natural Science Foundation of China(Nos.51972287 and 51502269)。
文摘Owing to their unique physicochemical,optical and electrical properties,two-dimensional(2D)MoS_(2) cocatalysts have been widely applied in designing and developing highly efficient composite photocatalysts for hydrogen generation under suitable light irradiation.In this review,we first elaborated on the fundamental aspects of 2D MoS_(2) cocatalysts to include the structural design principles,synthesis strategies,strengths and challenges.Subsequently,we thoroughly highlighted and discussed the modification strategies of 2D MoS_(2) H2-evolution cocatalysts,including doping heteroatoms(e.g.metals,non-metals,and co-doping),designing interfacial coupling morphologies,controlling the physical properties(e.g.thickness,size,structural defects or pores),exposing the reactive facets or edge sites,constructing cocatalyst heterojunctions,engineering the interfacial bonds and confinement effects.In the future,the forefront challenges in understanding and in precise controlling of the active sites at molecular level or atomic level should be carefully studied,while various potential mechanisms of photogenerated-electrons interactions should be proposed.The applications of MoS_(2) cocatalyst in the overall water splitting are also expected.This review may offer new inspiration for designing and constructing novel and efficient MoS_(2)-based composite photocatalysts for highly efficient photocatalytic hydrogen evolution.
基金financial support from the National Natural Science Foundation of China (21975129, 51902164)Natural Science Foundation of Jiangsu Province (BK20180777, BK20190759)+4 种基金Natural Science Foundation of Jiangsu Higher Education Institutions of China (18KJB430018, 19KJB430003)Scientific Research Foundation for Advanced Talents (CXL2018046)Science Innovation Foundation for Young Scientists (CX2018012)supported by Student’s Platform for Innovation and Entrepreneurship Training Program in Jiangsu Province (201810298029Z)Student’s Platform for Innovation and Entrepreneurship Training Program (2018NFUSPITP602)。
文摘Rational design and controllable synthesis of efficient electrocatalysts for water oxidation is of significant importance for the development of promising energy conversion systems, in particular integrated photoelectrochemical water splitting devices. Cobalt oxide(Co3O4) nanostructures with mixed valences(Ⅱ,Ⅲ)have been regarded as promising electrocatalysts for the oxygen evolution reaction(OER). They are able to promote catalytic support of OER but with only modest activity. Here, we demonstrate that the OER performance of cubic Co3O4 electrocatalyst is obviously improved when they are anchored on delaminated two-dimensional(2D) Ti3C2 MXene nanosheets. Upon activation the overpotential of the hybrid catalyst delivers 300 m V at a current density of 10 m A cm(2) in basic solutions, which is remarkably lower than those of Ti3C2 MXene and Co3O4 nanocubes. The strong interfacial electrostatic interactions between two components contribute to the exceptional catalytic performance and stability. The enhanced OER activity and facile synthesis make these Co3O4 nanocubes-decorated ultrathin 2D Ti3C2 MXene nanosheets useful for constructing efficient and stable electrodes for high-performance electrochemical water splitting.
基金This study was supported by Developed and Applied Funding of Tianjin Normal University(135202XK1702)Program for Innovative Research in the University of Tianjin(TD13-5077)+1 种基金National Natural Science Foundation of China(Number 21905202)Australian Research Council(ARC)through Discovery Early Career Researcher Awards(DECRA,DE170100871).
文摘Photoelectrochemical(PEC)water splitting is recognized as a sustainable strategy for hydrogen generation due to its abundant hydrogen source,utilization of inexhaustible solar energy,high-purity product,and environment-friendly process.To actualize a practical PEC water splitting,it is paramount to develop efficient,stable,safe,and low-cost photoelectrode materials.Recently,graphitic carbon nitride(g-C3N4)has aroused a great interest in the new generation photoelectrode materials because of its unique features,such as suitable band structure for water splitting,a certain range of visible light absorption,nontoxicity,and good stability.Some inherent defects of g-C3N4,however,seriously impair further improvement on PEC performance,including low electronic conductivity,high recombination rate of photogenerated charges,and limited visible light absorption at long wavelength range.Construction of g-C3N4-based nanosized heteroarrays as photoelectrodes has been regarded as a promising strategy to circumvent these inherent limitations and achieve the high-performance PEC water splitting due to the accelerated exciton separation and the reduced combination of photogenerated electrons/holes.Herein,we summarize in detail the latest progress of g-C3N4-based nanosized heteroarrays in PEC water-splitting photoelectrodes.Firstly,the unique advantages of this type of photoelectrodes,including the highly ordered nanoarray architectures and the heterojunctions,are highlighted.Then,different g-C3N4-based nanosized heteroarrays are comprehensively discussed,in terms of their fabrication methods,PEC capacities,and mechanisms,etc.To conclude,the key challenges and possible solutions for future development on g-C3N4-based nanosized heteroarray photoelectrodes are discussed.
基金financially supported by the National Natural Science Foundation of China(Nos.51404083 and 21273060)the Program for New Century Excellent Talents in Heilongjiang Provincial Universities(No.1253-NCET-010)the Natural Science Foundation of Heilongjiang Province,China(No.E2015065)
文摘In this study, CdS/g-C3N4 （CSCN） heterojunctions were in situ fabricated with a large amount of CdS nanoparticles anchored on g-C3N4 nanosheets, A wet chemical method was developed for the first time to determine the actual content of CdS in CSCN composites. X-ray diffraction （XRD）, Fourier transform infrared spectra （FFIR）, high-resolution transmission electron microscopy （HRTEM） and UV-vis diffuse reflectance spectra （DRS） were employed to characterize the composition, structure and optical prop- erty of CSCN composites. Based on the is0electric point （liP） analysis of g-C3N4, a conclusion was obtained on the combination mechanism between CdS nanoparticles and g-C3N4 nanosheets. The photocatalytic activity of CSCN composites was much better than those of individual CdS and g-C3N4 for the degrada- tion of azo dye Methyl Orange （MO） by 40 min adsorption in the dark followed by 15 min photocatalysis under visible light irradiation. After 5 cycles, CSCN composites still maintained high reactive activity with the MO degradation efficiency of 93.8%, exhibiting good photocatalytic stability. The Cd2~ concentration dissolved in the supernatant detected by atomic absorption spectroscopy （AAS） of CSCN composites was lower than that of pure CdS, implying that the photocorrosion of CdS could be suppressed via the combination with g-C3N4. Photoluminescence emission spectra （PL） results clearly revealed that the recombination of photogenerated electron-hole pairs in CSCN composites was effectively inhibited due to the formation of heterojunctions. Based on the band alignments of g-C3N4 and CdS, the possible photocatalvtic mechnism was discussed.
基金This work was jointly supported by the National Key Research and Development Program of China(Nos.2017YFA0206500 and 2018YFA0209103)the National Natural Science Foundation of China(Nos.21832003,21773111,51571110,and 21573107)the Fundamental Research Funds for the Central Universities(No.020514380126).
文摘As a choke point in water electrolysis,the oxygen evolution reaction(OER)suffers from the severe electrode polarization and large overpotential.Herein,the porous hierarchical hetero-(Nis Fe)FeN/Ni catalysts are in situ constructed for the eficient electrocatalytic OER.X-ray absorption fine structure characterizations reveal the strong Ni-Fe bimetallic interaction in(Niz Fex)FeN/Ni.Theoretical study indicates the heterojunction and bimetallic interaction decrease the free-energy change for the rate-limiting step of the OER and the overpotential thereof.In addition,the high conductivity and porous hierarchical morphology favor the electron transfer,electrolyte access and O2 release.Consequently,the optimized catalyst achieves a low overpotential of 223 mV at 10 mA.cm^-2,a small Tafel slope of 68 mV:dec^-1,and a high stability.The excellent performance of the optimized catalyst is also demonstrated by the overall water electrolysis with a low working voltage and high Faradaic efficiency.Moreover,the correlation between the structure and performance is well established by the experimental characterizations and theoretical calculations,which confirms the origin of the OER activity from the surface metal oxyhydroxide in situ generated upon applying the current.This study suggests a promising approach to the advanced OER electrocatalysts for practical applications by constructing the porous hierarchical metal-compound/metal heterojunctions.
基金This work was supported by the National Basic Research Program of China （Nos. 2012CB932400 and 2013CB933500）, the Major Research Plan of the National Natural Science Foundation of China （Nos. 91233110 and 91333208）, the National Na~ral Science Foundation of China （No. 61422403）, the Natural Science Foundation of Jiangsu Province （No. BK20140332）, and a Project Funded by the Priority Academic Program Development of Jiangsu Higher Education Institutions （PAPD）. This work was also supported by QinLan Project.
文摘As one of the most important semiconductor materials, silicon （Si） has been widely used in current energy and optoelectronic devices, such as solar cells and photodetectors. However, the traditional Si p-n junction solar cells need complicated fabrication processes, leading to the high cost of Si photovoltaic devices. The wide applications of Si-based photodetectors are also hampered by their low sensitivity to ultraviolet and infrared light. Recently, two-dimensional （2D） layered materials have emerged as a new material system with tremendous potential for future energy and optoelectronic applications. The combination of Si with 2D layered materials represents an innovative approach to construct high-performance optoelectronic devices by harnessing the complementary advantages of both materials. In this review, we summarize the recent advances in 2D layered material/Si heterojunctions and their applications in photovoltaic and optoelectronic devices. Finally, the outlook and challenges of 2D layered material/Si heterojunctions for high-performance device applications are presented.
基金supprted by the National Natural Science Foundation of China(51672089,51672099)Specical Funding on Applied Science and Technology in Guangdong(2017B020238005)the State Key Laboratory of Advanced Technology for Material Synthesis and Processing(Wuhan University of Technology)(2015-KF-7)~~
文摘Photocatalysis is believed to be one of the best methods to realize sustainable H2 production. However, achieving this through heterogeneous photocatalysis still remains a great challenge owing to the absence of active sites, sluggish surface reaction kinetics, insufficient charge separation, and a high thermodynamic barrier. Therefore, cocatalysts are necessary and of great significance in boosting photocatalytic H2 generation. This review will focus on the promising and appealing low-cost Ni-based H2-generation cocatalysts as the alternatives for the high-cost and low-abundance noble metal cocatalysts. Special emphasis has been placed on the design principle, modification strategies for further enhancing the activity and stability of Ni-based cocatalysts, and identification of the exact active sites and surface reaction mechanisms. Particularly, four types of modification strategies based on increased light harvesting, enhanced charge separation, strengthened interface interaction, and improved electrocatalytic activity have been thoroughly discussed and compared in detail. This review may open a new avenue for designing highly active and durable Ni-based cocatalysts for photocatalytic H2 generation.
基金This work was supported by the Key Project of Natural Science Foundation of Shandong Province （No. ZR2013EMZ001）, the Science and Technology Development Plan Project of Shandong Province （No. 2014GSF117015）, the National Basic Research Program of China （No. 2013CB632401） and the National Natural Science Foundation of China （No. 51402145）. This work was also supported by the U.S. Department of Energy under Contract DE-AC0206CH11357 with the main support provided by the Vehicle Technologies Office, Department of Energy （DOE） Office of Energy Efficiency and Renewable Energy （EERE）.
文摘Novel SnO2-x/g-C3N4 heterojunction nanocomposites composed of reduced SnO2 nanoparticles and exfoliated g-CBN4 nanosheets were prepared by a convenient one-step pyrolysis method. The structural, morphological, and optical properties of the as-prepared nanocomposites were characterized in detail, indicating that the aggregation of g-C3N4 nanosheets was prevented by small, well-dispersed SnO2_x nanoparticles. The ultraviolet-visible spectroscopy absorption bands of the nanocomposites were shifted to a longer wavelength region than those exhibited by pure SnO2 or g-CgN4. The charge transfer and recombination processes occurring in the nanocomposites were investigated using linear scan voltammetry and electrochemical impedance spectroscopy. Under 30-W visible-light-emitting diode irradiation, the heterojunction containing 27.4 wt.% SnO2-x exhibited the highest photocurrent density of 0.0468 mA.cm-2, which is 33.43 and 5.64 times larger than that of pure SnO2 and g-C3N4, respectively. The photocatalytic activity of the heterojunction material was investigated by degrading rhodamine B under irradiation from the same light source. Kinetic study revealed a promising degradation rate constant of 0.0226 min^-1 for the heterojunction containing 27.4 wt.% SnO2-x, which is 32.28 and 5.79 times higher than that of pure SnO2 and g-C3N4, respectively. The enhanced photoelectrochemical and photocatalytic performances of the nanocomposite may be due to its appropriate SnO2x content and the compact structure of the junction between the SnO2-x nanoparticles and the g-C3N4 nanosheets, which inhibits the recombination of photogenerated electrons and holes.
基金support from the National Basic Research Program of China(No.2016YFA0200101)the National Natural Science Foundation of China(Nos.21733001 and 21525310)Boya Postdoctoral Fellowship.
文摘The formation of heterojunction within solid-state devices enables them with eventually high performances,but provides a challenge for material synthesis and device fabrication because strict conditions such as lattice match are needed.Herein,we show a facile method to fabricate a van der Waals(vdW)heterojunction between two-dimensional(2D)bismuth oxyselenide(Bi2O2Se)and graphene,during which the graphene is directly transferred to the Bi2O2Se and served as a lowcontract-resistant electrode with small work function mismatch(~50 meV).As an optoelectronic device,the Bi2O2Se/graphene vdW heterojunction allows for the efficient sensing toward 1200-nm incident laser.Regarding the application of fieldeffect transistors(FETs),the short-channel(50 nm)sample can be synthesized by utilizing these two 2D materials(ie,channel:Bi2O2Se;drain/source terminal:graphene)and the n-type characteristic can be observed with the accordant field modulation.It is confirmed that we show a simple way to prepare the vdW heterojunction which is aiming to the high-performance applications among optoelectronics and FETs.
基金This work was supported by the National Natural Science Foundation of China （Nos. 21401079, 21501069, and 21671081）, Fundamental Research Funds for the Central Universities （No. JUSRP51626B）, and Natural Science Foundation of Jiangsu Province （Nos. BK20140158 and BK20161128）.
文摘The traditional single material with two-dimensional （2D） biomimetic moth-eye structures is limited by its narrowband antireflection and single functional capability. To overcome these disadvantages, we exploited wet etching and hydrothermal synthesis coupled with chemical oxidation for fabricating a three- dimensional （3D） biomimetic moth-eye coating with ternary materials （polypyrrole nanoparticles, TiO2 nanorods, and Si micropyramids, i.e., PPy/TiOa/Si-p）. This coating reduced the reflectivity to 〈4% at wavelengths ranging from 200 to 2,300 nm and exhibited remarkable superhydrophilidty with a low water contact angle of 1.8°. Moreover, the composite coating had double p-n heterojunctions, allowing the high-efficiency separation of photogenerated carriers. The photo- current density of PPy/TiO2/Si-p was more than three times higher than that of TiO2/Si-p at a positive potential of 1.5 V. The proposed method provides a means to enhance solar energy conversion.
基金financially supported by the National Natural Science Foundation of China(Nos.21663027,21808189)the Fundamental Research Funds for the Central Universities of Chang’an University(No.300102299304)the Natural Science Basic Research Fund of Shaanxi Province(No.2020JZ20)。
文摘Photoelectrochemical(PEC)technology is considered to be a promising approach for solar-driven hydrogen production with zero emissions.Bismuth vanadate(BiVO_(4))is a kind of photocatalytic material with strong photoactivity in the visible light region and appropriate band gap for PEC water splitting.However,the solar-to-hydrogen efficiency(STH)of BiVO_(4)is far away from the 10%target needed for practical application due to its poor charge separation ability.Therefore,this review attempts to summarize the strategies for improving the photocurrent density and especially hydrogen production of BiVO_(4)materials through PEC techniques in the last three years,such as doping nonmetal and metal elements,depositing noble metals,constructing heterojunctions,coupling with carbon and metalorganic framework(MOF)materials to further enhance the PEC performance of BiVO_(4)photoanode.This review aims to serve as a general guideline to fabricate highly efficient BiVO_(4)-based materials for PEC water splitting.
基金supported by the National Key Research and Development Program of China(2018YFB1502003)the National Natural Science Foundation of China(51961165103)supported by the National Program for Support of Top-notch Young Professionals and‘‘The Youth Innovation Team of Shaanxi Universities”。
文摘Carbon nitride-based photocatalysts hold an enormous potential in producing hydrogen.A strategy to simultaneously create isotype heterojunctions and active sites in highly-crystallized carbon nitride is anticipated to significantly boost the photocatalytic activity,but is yet to be realized.Herein,we find that cobalt salt added in the ionothermal synthesis can promote the phase transition of heptazine-based crystalline carbon nitride(CCN)to triazine-based poly(triazine imide)(PTI),rendering the creation of singleatom cobalt coordinated isotype CCN/PTI heterojunction.Co-CCN/PTI exhibits an appreciable apparent quantum yield of 20.88%at 425 nm for photocatalytic hydrogen production with a rate achieving3538μmol h^(-1)g^(-1)(λ>420 nm),which is 4.8 times that of CCN and 27.6 times that of PTI.The high photocatalytic activity is attributed to the Type II isotype highly-crystallized CCN/PTI heterojunction for promoting charge carrier migration,and the single-atom Co sites for accelerating surface oxidation reaction.
基金supported by the National Natural Science Foundation of China(grant nos.21975026 and 22005033)the National Postdoctoral Program of China(no.BX20180037)+1 种基金China Postdoctoral Science Foundation(no.2018M640077)the Beijing Institute of Technology Research Fund Program for Young Scholars(no.XSQD-202108005).
文摘Developing effective strategies to improve the initial Coulombic efficiency(ICE)and cycling stability of hard carbon(HC)anodes for sodium-ion batteries is the key to promoting the commercial application of HC.In this paper,homotype heterojunctions are designed on HC to induce the generation of stable solid electrolyte interfaces,which can effectively increase the ICE of HC from 64.7%to 81.1%.The results show that using a simple surface engineering strategy to construct a homotypic amorphous Al_(2)O_(3) layer on the HC could shield the active sites,and further inhibit electrolyte decomposition and side effects occurrence.Particularly,due to the suppression of continuous decomposition of NaPF 6 in ester-based electrolytes,the accumulation of NaF could be reduced,leading to the formation of thinner and denser solid electrolyte interface films and a decrease in the interface resistance.The HC anode can not only improve the ICE but elevate its sodium storage performance based on this homotype heterojunction composed of HC and Al_(2)O_(3).The optimized HC anode exhibits an outstanding reversible capacity of 321.5mAhg^(−1) at 50mAg^(−1).The cycling stability is also improved effectively,and the capacity retention rate is 86.9%after 2000 cycles at 1Ag^(−1) while that of the untreated HC is only 52.6%.More importantly,the improved sodium storage behaviors are explained by electrochemical kinetic analysis.
基金Acknowledgements This work was supported in part by National Basic Research Program of China （Nos. 2013CBA01604 and 2015CB921600）, National Natural Science Foundation of China （Nos. 61325020, 61261160499, 11274154, and 61521001）, Research Grant Council of Hong Kong （No. SARN_CUHK405/12）, Collaborative Innovation Center of Solid-State Lighting and Energy-Saving Electronics, ＂Jiangsu Shuangchuang＂ program and ＂Jiangsu Shuangchuang Team＂ Program.
文摘Van der Waals （vdW） heterojunctions based on two-dimensional （2D） atomic crystals have been extensively studied in recent years. Herein, we show that both vertical and lateral vdW heterojunctions can be realized with layered molecular crystals using a two-step physical vapor transport （PVT） process. Both types of heterojunctions show clean and sharp interfaces without phase mixing under atomic force microscopy （AFM）. They also exhibit a strong interfacial built-in electric field similar to that of their inorganic counterparts. These heterojunctions have greater potential for device applications than individual materials. The lateral heterojunction （LHJ） devices show rectifying characteristics due to the asymmetric energy barrier for holes at the interface, while the vertical heterojunction （VHJ） devices behave like metal-insulator-semiconductor tunnel junctions, with pronounced negative differential conductance （NDC）. Our work extends the concept of vdW heterojunctions to molecular materials, which can be generalized to other layered organic semiconductors （OSCs） to obtain new device functionalities.
基金This work was supported by the National Natural Science Foundation of China (No. 10274108)the National "973" Project of China (No. 2004CB719804)the National "863" Project of China (No. 2003AA311022)the Natural Science Foundation of Guangdong Province of China.
文摘A photonic heterostructure with multi-channel and sharp angular defect modes by combining two different one-dimensional defective photonic crystals is proposed. The filters designed on the basis of this heterostructure possess both functions of multi-channel narrow band filtering and sharp angular filtering. The channels, channel interval, and number of channels can be tuned by adjusting the geometric and physical parameters of the heterostuctures. This kind of filters will benefit the development of multi-channel interstellar or atmosphere optical communication.
