We use laser-scanning nonlinear imaging microscopy in atomically thin transition metal dichalcogenides(TMDs)to reveal information on the crystalline orientation distribution,within the 2D lattice.In particular,we perf...We use laser-scanning nonlinear imaging microscopy in atomically thin transition metal dichalcogenides(TMDs)to reveal information on the crystalline orientation distribution,within the 2D lattice.In particular,we perform polarization-resolved second-harmonic generation(PSHG)imaging in a stationary,raster-scanned chemical vapor deposition(CVD)-grown WS2 flake,in order to obtain with high precision a spatially resolved map of the orientation of its main crystallographic axis(armchair orientation).By fitting the experimental PSHG images of sub-micron resolution into a generalized nonlinear model,we are able to determine the armchair orientation for every pixel of the image of the 2D material,with further improved resolution.This pixel-wise mapping of the armchair orientation of 2D WS2 allows us to distinguish between different domains,reveal fine structure,and estimate the crystal orientation variability,which can be used as a unique crystal quality marker over large areas.The necessity and superiority of a polarization-resolved analysis over intensity-only measurements is experimentally demonstrated,while the advantages of PSHG over other techniques are analysed and discussed.展开更多
In perovskite solar cells(PSCs),the inherent defects of perovskite film and the random distribution of excess lead iodide(PbI_(2))prevent the improvement of efficiency and stability.Herein,natural cellulose is used as...In perovskite solar cells(PSCs),the inherent defects of perovskite film and the random distribution of excess lead iodide(PbI_(2))prevent the improvement of efficiency and stability.Herein,natural cellulose is used as the raw material to design a series of cellulose derivatives for perovskite crystallization engineering.The cationic cellulose derivative C-Im-CN with cyano-imidazolium(Im-CN)cation and chloride anion prominently promotes the crystallization process,grain growth,and directional orientation of perovskite.Meanwhile,excess PbI_(2)is transferred to the surface of perovskite grains or formed plate-like crystallites in local domains.These effects result in suppressing defect formation,decreasing grain boundaries,enhancing carrier extraction,inhibiting non-radiative recombination,and dramatically prolonging carrier lifetimes.Thus,the PSCs exhibit a high power conversion efficiency of 24.71%.Moreover,C-Im-CN has multiple interaction sites and polymer skeleton,so the unencapsulated PSCs maintain above 91.3%of their initial efficiencies after 3000 h of continuous operation in a conventional air atmosphere and have good stability under high humidity conditions.The utilization of biopolymers with excellent structure-designability to manage the perovskite opens a state-of-the-art avenue for manufacturing and improving PSCs.展开更多
Captured by the environmental and economic value,the recycling of spent lithium iron phosphate(LFP)batteries has attracted numerous attentions.However,hydrometallurgical method still suffers from complex process,and h...Captured by the environmental and economic value,the recycling of spent lithium iron phosphate(LFP)batteries has attracted numerous attentions.However,hydrometallurgical method still suffers from complex process,and hydrothermal method is limited by morphology control,ascribed to the strong polarity of water.Herein,supported by ethanol as crystal surface modifier,the regular(010)orientation and short b-axis are effectively tailored for regenerated LFP.As Li-storage cathode,the capacities of as-optimized LFP could reach up to 157.07 mA h g^(-1)at 1 C,and the stable capacity of 150.50 mA h g^(-1)could be remained with retention of 93.48%after 400 cycles at 1 C.Even at 10 C,their capacity could be still kept about 119.3 m A h g^(-1).Assisted by the detail analysis of adsorption energy,the clear growth mechanism is proposed,the lowest adsorbing energy(-4.66 eV)of ethanol on(010)crystal plane renders the ordered growth along(010)crystal plane.Given this,the work is expected to shed light on the tailoring mechanism of internal plane about regenerated materials,whilst providing effective strategies for highperformance regenerated LFP.展开更多
Growth of high-quality Nb_(3)Sn thin films for superconducting radiofrequency(SRF)applications using the vapor diffusion method requires a uniform distribution of tin nuclei on the niobium(Nb)surface.This study examin...Growth of high-quality Nb_(3)Sn thin films for superconducting radiofrequency(SRF)applications using the vapor diffusion method requires a uniform distribution of tin nuclei on the niobium(Nb)surface.This study examines the mechanism underlying the observed non-uniform distribution of tin nuclei with tin chloride SnCl_(2).Electron backscatter diffraction(EBSD)analysis was used to examine the correlation between the nucleation behavior and orientation of niobium grains in the substrate.The findings of the density functional theory(DFT)simulation are in good agreement with the experimental results,showing that the non-uniform distribution of tin nuclei is the result of the adsorption energy of SnCl_(2)molecules by varied niobium grain orientations.Further analysis indicated that the surface roughness and grain size of niobium also played significant roles in the nucleation behavior.This study provides valuable insights into enhancing the surface pretreatment of niobium substrates during the growth of Nb_(3)Sn thin films using the vapor diffusion method.展开更多
Crystal orientation influences the morphological stability of solid–liquid interface during directional solidification of alloy, resulting in the variation of solidified microstructure. In this paper, the morphologic...Crystal orientation influences the morphological stability of solid–liquid interface during directional solidification of alloy, resulting in the variation of solidified microstructure. In this paper, the morphological evolution near grain boundary grooves（GBGs） with different crystal orientations in a dilute succinonitrile alloy under low temperature gradient and interface velocity is observed in situ. Under experimental conditions, the macroscopic solid–liquid interface is planar and keeps stable, while in GBGs there emerge protrusion and undulation. It is found that the morphological stability of GBG is dependent on crystal orientation. Specifically, for succinonitrile with a body-centered cubic crystal structure, GBGs around the 100 crystal orientation keep stable, while those apart from the 100 crystal orientation become unstable under the same conditions. So it is concluded that 100 crystal orientation favors the morphological stability of GBG.展开更多
The last several years have witnessed the prosperous development of zinc-ion batteries(ZIBs),which are considered as a promising competitor of energy storage systems thanks to their low cost and high safety.However,th...The last several years have witnessed the prosperous development of zinc-ion batteries(ZIBs),which are considered as a promising competitor of energy storage systems thanks to their low cost and high safety.However,the reversibility and availability of this system are blighted by problems such as uncontrollable dendritic growth,hydrogen evolution,and corrosion passivation on anode side.A functionally and structurally well-designed anode current collectors(CCs)is believed as a viable solution for those problems,with a lack of summarization according to its working mechanisms.Herein,this review focuses on the challenges of zinc anode and the mechanisms of modified anode CCs,which can be divided into zincophilic modification,structural design,and steering the preferred crystal facet orientation.The possible prospects and directions on zinc anode research and design are proposed at the end to hopefully promote the practical application of ZIBs.展开更多
Sb_(2)Se_(3)solar cells have achieved a power conversion efficiency(PCE)of over 10%.However,the serious open-circuit voltage deficit(VOC-deificit),induced by the hard-to-control crystal orientation and heterojunction ...Sb_(2)Se_(3)solar cells have achieved a power conversion efficiency(PCE)of over 10%.However,the serious open-circuit voltage deficit(VOC-deificit),induced by the hard-to-control crystal orientation and heterojunction interface reaction,limits the PCE of vapor transport deposition(VTD)processed Sb_(2)Se_(3)solar cells.To overcome the VOC-deficit problem of VTD processed Sb_(2)Se_(3)solar cells,herein,an in-situ bandgap regulation strategy is innovatively proposed to prepare a wide band gap Sb2(S,Se)3seed layer(WBSL)at CdS/Sb_(2)Se_(3)heterojunction interface to improve the PCE of Sb_(2)Se_(3)solar cells.The analysis results show that the introduced Sb2(S,Se)3seed layer can enhance the[001]orientation of Sb_(2)Se_(3)thin films,broaden the band gap of heterojunction interface,and realize a"Spike-like"conduction band alignment with ΔE_(c)=0.11 eV.In addition,thanks to the suppressed CdS/Sb_(2)Se_(3)interface reaction after WBSL application,the depletion region width of Sb_(2)Se_(3)solar cells is widened,and the quality of CdS/Sb_(2)Se_(3)interface and the carrier transporting performance of Sb_(2)Se_(3)solar cells are significantly improved as well.Moreover,the harmful Se vacancy defects near the front interface of Sb_(2)Se_(3)solar cells can be greatly diminished by WBSL.Finally,the PCE of Sb_(2)Se_(3)solar cells is improved from 7.0%to 7.6%;meanwhile the VOCis increased to 466 mV which is the highest value for the VTD derived Sb_(2)Se_(3)solar cells.This work will provide a valuable reference for the interface and orientation regulation of antimony-based chalcogenide solar cells.展开更多
文摘We use laser-scanning nonlinear imaging microscopy in atomically thin transition metal dichalcogenides(TMDs)to reveal information on the crystalline orientation distribution,within the 2D lattice.In particular,we perform polarization-resolved second-harmonic generation(PSHG)imaging in a stationary,raster-scanned chemical vapor deposition(CVD)-grown WS2 flake,in order to obtain with high precision a spatially resolved map of the orientation of its main crystallographic axis(armchair orientation).By fitting the experimental PSHG images of sub-micron resolution into a generalized nonlinear model,we are able to determine the armchair orientation for every pixel of the image of the 2D material,with further improved resolution.This pixel-wise mapping of the armchair orientation of 2D WS2 allows us to distinguish between different domains,reveal fine structure,and estimate the crystal orientation variability,which can be used as a unique crystal quality marker over large areas.The necessity and superiority of a polarization-resolved analysis over intensity-only measurements is experimentally demonstrated,while the advantages of PSHG over other techniques are analysed and discussed.
基金supported by the National Natural Science Foundation of China(No.52173292 and U2004211)the Youth Innovation Promotion Association CAS(No.2018040).
文摘In perovskite solar cells(PSCs),the inherent defects of perovskite film and the random distribution of excess lead iodide(PbI_(2))prevent the improvement of efficiency and stability.Herein,natural cellulose is used as the raw material to design a series of cellulose derivatives for perovskite crystallization engineering.The cationic cellulose derivative C-Im-CN with cyano-imidazolium(Im-CN)cation and chloride anion prominently promotes the crystallization process,grain growth,and directional orientation of perovskite.Meanwhile,excess PbI_(2)is transferred to the surface of perovskite grains or formed plate-like crystallites in local domains.These effects result in suppressing defect formation,decreasing grain boundaries,enhancing carrier extraction,inhibiting non-radiative recombination,and dramatically prolonging carrier lifetimes.Thus,the PSCs exhibit a high power conversion efficiency of 24.71%.Moreover,C-Im-CN has multiple interaction sites and polymer skeleton,so the unencapsulated PSCs maintain above 91.3%of their initial efficiencies after 3000 h of continuous operation in a conventional air atmosphere and have good stability under high humidity conditions.The utilization of biopolymers with excellent structure-designability to manage the perovskite opens a state-of-the-art avenue for manufacturing and improving PSCs.
基金supported by the National Natural Science Foundation of China(52374290,52374288 and 52204298)the Innovation-driven Program of Central South University(2023CXQD009)+3 种基金the Hunan Provincial Innovation Foundation for Postgraduate(2024ZZTS0059)the Young Elite Scientists Sponsorship Program by China Association for Science and Technology(2022QNRC001)the National Key Research and Development Program of China(2022YFC3900805-4/7)the Hunan Provincial Education Office Foundation of China(21B0147)。
文摘Captured by the environmental and economic value,the recycling of spent lithium iron phosphate(LFP)batteries has attracted numerous attentions.However,hydrometallurgical method still suffers from complex process,and hydrothermal method is limited by morphology control,ascribed to the strong polarity of water.Herein,supported by ethanol as crystal surface modifier,the regular(010)orientation and short b-axis are effectively tailored for regenerated LFP.As Li-storage cathode,the capacities of as-optimized LFP could reach up to 157.07 mA h g^(-1)at 1 C,and the stable capacity of 150.50 mA h g^(-1)could be remained with retention of 93.48%after 400 cycles at 1 C.Even at 10 C,their capacity could be still kept about 119.3 m A h g^(-1).Assisted by the detail analysis of adsorption energy,the clear growth mechanism is proposed,the lowest adsorbing energy(-4.66 eV)of ethanol on(010)crystal plane renders the ordered growth along(010)crystal plane.Given this,the work is expected to shed light on the tailoring mechanism of internal plane about regenerated materials,whilst providing effective strategies for highperformance regenerated LFP.
基金supported by the National Natural Science Foundation of China(No.12175283)Youth Innovation Promotion Association of Chinese Academy of Sciences(2020410)Advanced Energy Science and Technology Guangdong Laboratory(HND20TDSPCD,HND22PTDZD).
文摘Growth of high-quality Nb_(3)Sn thin films for superconducting radiofrequency(SRF)applications using the vapor diffusion method requires a uniform distribution of tin nuclei on the niobium(Nb)surface.This study examines the mechanism underlying the observed non-uniform distribution of tin nuclei with tin chloride SnCl_(2).Electron backscatter diffraction(EBSD)analysis was used to examine the correlation between the nucleation behavior and orientation of niobium grains in the substrate.The findings of the density functional theory(DFT)simulation are in good agreement with the experimental results,showing that the non-uniform distribution of tin nuclei is the result of the adsorption energy of SnCl_(2)molecules by varied niobium grain orientations.Further analysis indicated that the surface roughness and grain size of niobium also played significant roles in the nucleation behavior.This study provides valuable insights into enhancing the surface pretreatment of niobium substrates during the growth of Nb_(3)Sn thin films using the vapor diffusion method.
基金Project supported by the National Natural Science Foundation of China(Grant No.51271213)the National Basic Research Program of China(Grant No.2011CB610402)+1 种基金China Postdoctoral Science Foundation(Grant No.2013M542384)the Specialized Research Fund for the Doctoral Program of Higher Education of China(Grant No.20116102110016)
文摘Crystal orientation influences the morphological stability of solid–liquid interface during directional solidification of alloy, resulting in the variation of solidified microstructure. In this paper, the morphological evolution near grain boundary grooves（GBGs） with different crystal orientations in a dilute succinonitrile alloy under low temperature gradient and interface velocity is observed in situ. Under experimental conditions, the macroscopic solid–liquid interface is planar and keeps stable, while in GBGs there emerge protrusion and undulation. It is found that the morphological stability of GBG is dependent on crystal orientation. Specifically, for succinonitrile with a body-centered cubic crystal structure, GBGs around the 100 crystal orientation keep stable, while those apart from the 100 crystal orientation become unstable under the same conditions. So it is concluded that 100 crystal orientation favors the morphological stability of GBG.
基金supported by the National Natural Science Foundation of China(Grant Nos.51874110 and 51604089)Natural Science Foundation of Heilongjiang Province(YQ2021B004)Open Project of State Key Laboratory of Urban Water Resource and Environment(Grant No.QA202138).
文摘The last several years have witnessed the prosperous development of zinc-ion batteries(ZIBs),which are considered as a promising competitor of energy storage systems thanks to their low cost and high safety.However,the reversibility and availability of this system are blighted by problems such as uncontrollable dendritic growth,hydrogen evolution,and corrosion passivation on anode side.A functionally and structurally well-designed anode current collectors(CCs)is believed as a viable solution for those problems,with a lack of summarization according to its working mechanisms.Herein,this review focuses on the challenges of zinc anode and the mechanisms of modified anode CCs,which can be divided into zincophilic modification,structural design,and steering the preferred crystal facet orientation.The possible prospects and directions on zinc anode research and design are proposed at the end to hopefully promote the practical application of ZIBs.
基金supported by the National Natural Science Foundation of China(62305064)the Research Start-up Fund for Young Teachers of Fuzhou University(602592)+1 种基金the Young and Middleaged Teacher Education Research Project of Fujian Province(JAT220011)the Fujian Science&Technology Innovation Laboratory Optoelectronic Information of China(Grant No.2021ZZ124).
文摘Sb_(2)Se_(3)solar cells have achieved a power conversion efficiency(PCE)of over 10%.However,the serious open-circuit voltage deficit(VOC-deificit),induced by the hard-to-control crystal orientation and heterojunction interface reaction,limits the PCE of vapor transport deposition(VTD)processed Sb_(2)Se_(3)solar cells.To overcome the VOC-deficit problem of VTD processed Sb_(2)Se_(3)solar cells,herein,an in-situ bandgap regulation strategy is innovatively proposed to prepare a wide band gap Sb2(S,Se)3seed layer(WBSL)at CdS/Sb_(2)Se_(3)heterojunction interface to improve the PCE of Sb_(2)Se_(3)solar cells.The analysis results show that the introduced Sb2(S,Se)3seed layer can enhance the[001]orientation of Sb_(2)Se_(3)thin films,broaden the band gap of heterojunction interface,and realize a"Spike-like"conduction band alignment with ΔE_(c)=0.11 eV.In addition,thanks to the suppressed CdS/Sb_(2)Se_(3)interface reaction after WBSL application,the depletion region width of Sb_(2)Se_(3)solar cells is widened,and the quality of CdS/Sb_(2)Se_(3)interface and the carrier transporting performance of Sb_(2)Se_(3)solar cells are significantly improved as well.Moreover,the harmful Se vacancy defects near the front interface of Sb_(2)Se_(3)solar cells can be greatly diminished by WBSL.Finally,the PCE of Sb_(2)Se_(3)solar cells is improved from 7.0%to 7.6%;meanwhile the VOCis increased to 466 mV which is the highest value for the VTD derived Sb_(2)Se_(3)solar cells.This work will provide a valuable reference for the interface and orientation regulation of antimony-based chalcogenide solar cells.
