Perovskite solar cells(PSCs)have attracted aggressive attention in the photovoltaic field in light of the rapid increasing power conversion efficiency.However,their large-scale application and commercialization are li...Perovskite solar cells(PSCs)have attracted aggressive attention in the photovoltaic field in light of the rapid increasing power conversion efficiency.However,their large-scale application and commercialization are limited by the toxicity issue of lead(Pb).Among all the lead-free perovskites,tin(Sn)-based perovskites have shown potential due to their low toxicity,ideal bandgap structure,high carrier mobility,and long hot carrier lifetime.Great progress of Sn-based PSCs has been realized in recent years,and the certified efficiency has now reached over 14%.Nevertheless,this record still falls far behind the theoretical calculations.This is likely due to the uncontrolled nucleation states and pronounced Sn(Ⅳ)vacancies.With insights into the methodologies resolving both issues,ligand engineering-assisted perovskite film fabrication dictates the state-of-the-art Sn-based PSCs.Herein,we summarize the role of ligand engineering during each state of film fabrication,ranging from the starting precursors to the ending fabricated bulks.The incorporation of ligands to suppress Sn~(2+)oxidation,passivate bulk defects,optimize crystal orientation,and improve stability is discussed,respectively.Finally,the remained challenges and perspectives toward advancing the performance of Sn-based PSCs are presented.We expect this review can draw a clear roadmap to facilitate Sn-based PSCs via ligand engineering.展开更多
Cd-based Cs_(7)Cd_(3)Br_(13)perovskites,featuring both tetrahedral and octahedral polyhedral structures,have garnered significant acclaim for their efficient luminescent performance achieved through multi-exciton stat...Cd-based Cs_(7)Cd_(3)Br_(13)perovskites,featuring both tetrahedral and octahedral polyhedral structures,have garnered significant acclaim for their efficient luminescent performance achieved through multi-exciton state regulation by doping.However,it remains controversial whether the doping sites are in the octahedra or tetrahedra of Cs_(7)Cd_(3)Br_(13).To address this,we introduced Pb^(2+)and Sb^(3+)ions and,supported by experimental and theoretical evidence,demonstrated that these ions preferentially occupy the octahedra.Among them,Pb^(2+)ions single doping achieves a near-unity photoluminescence quantum yield of 93.7%,which results in excellent X-ray scintillation performance,high light yield of 41,772 photon MeV^(-1),and a low detection limit of 29.78 nGyairs-1.Moreover,this incorporation of Pb^(2+)and Sb^(3+)enabled an exciton state regulation strategy,resulting in standard white light emission with CIE chromaticity coordinates of(0.33,0.33).Additionally,a multifaceted optical anticounterfeiting and information encryption scheme was designed based on the differences in optical properties caused by the different sensitivities of[PbBr6]4-octahedron and[SbBr6]3-octahedron to temperature and excitation wavelengths.These diverse photoluminescence characteristics provide new insights and practical demonstrations for advanced X-ray imaging,lighting,optical encryption,and anticounterfeiting technologies.展开更多
An imine-based nitrogen-rich covalent-organic framework(COF)was successfully synthesized using two tri-angular building units under solvothermal reaction condition.The gas adsorption properties of the obtained micro-p...An imine-based nitrogen-rich covalent-organic framework(COF)was successfully synthesized using two tri-angular building units under solvothermal reaction condition.The gas adsorption properties of the obtained micro-porous nitrogen-rich COF were investigated.The results indicated that the activated COF material presented good up take capabilities of CO_(2) and CH_(4) at 61.2 and 43.4 cm^(3)·g^(−1)at 1 atm and 273 K,respectively,showing its applica-tion potential in selective gas capture and separation.展开更多
Nucleation is a critical stage during the crystallization process,determining the attributes of the crystalline products.Due to the complicated and microscopic characteristics of the molecular assembly process,the nuc...Nucleation is a critical stage during the crystallization process,determining the attributes of the crystalline products.Due to the complicated and microscopic characteristics of the molecular assembly process,the nucleation mechanism has not yet been fully comprehended.In this study,the molecular self-assembly of 4-bromopyrazole(BMPZ)in various solvents and its relation with nucleation kinetics were investigated by the experiment and molecule simulation.Firstly,Fourier transform infrared spectroscopy,nuclear magnetic resonance spectroscopy,and mass spectroscopy were employed to explore and determine the existed forms of BMPZ molecules in solution.It was unveiled that the BMPZ molecules assembly behavior showed an individual feature.Afterward,the nucleation kinetics was determined by statistical probability distribution method,and the parameters associated with the nucleation process were derived from classical nucleation theory,further associating with the nucleation kinetics.Solution chemistry,molecule simulation,and nucleation kinetics exposed that BMPZ assembly forms could act as the growth unit of the nucleation,and nucleation kinetics was chiefly governed by the interface-transfer process.展开更多
基金supported by the National Natural Science Foundation of China(61935016,62275213 and 62205264),the National Natural Science Foundation of China(21961160720)the Fundamental Research Funds for Xi'an Jiaotong University(xzy012022092,xzd012022003 and xzy022022057)+1 种基金the National Key Research and Development Program of China(2022YFB3803300)the open research fund of Songshan Lake Materials Laboratory(2021SLABFK02)。
文摘Perovskite solar cells(PSCs)have attracted aggressive attention in the photovoltaic field in light of the rapid increasing power conversion efficiency.However,their large-scale application and commercialization are limited by the toxicity issue of lead(Pb).Among all the lead-free perovskites,tin(Sn)-based perovskites have shown potential due to their low toxicity,ideal bandgap structure,high carrier mobility,and long hot carrier lifetime.Great progress of Sn-based PSCs has been realized in recent years,and the certified efficiency has now reached over 14%.Nevertheless,this record still falls far behind the theoretical calculations.This is likely due to the uncontrolled nucleation states and pronounced Sn(Ⅳ)vacancies.With insights into the methodologies resolving both issues,ligand engineering-assisted perovskite film fabrication dictates the state-of-the-art Sn-based PSCs.Herein,we summarize the role of ligand engineering during each state of film fabrication,ranging from the starting precursors to the ending fabricated bulks.The incorporation of ligands to suppress Sn~(2+)oxidation,passivate bulk defects,optimize crystal orientation,and improve stability is discussed,respectively.Finally,the remained challenges and perspectives toward advancing the performance of Sn-based PSCs are presented.We expect this review can draw a clear roadmap to facilitate Sn-based PSCs via ligand engineering.
基金funded by the Jinan Central Hospital Collaboration(1190022050)Foundation for Innovative Research Groups of the National Natural Science Foundation of China(22205233,62374103,62374104,and 62405165)+3 种基金Basic and Applied Basic Research Foundation of Guangdong Province(2024A1515010926)Taishan Scholar Foundation of Shandong Province of Shandong Province(tsqn202312005)Postdoctoral Innovative Projects of Shandong Province(202400321)China Postdoctoral Science Foundation(2024M751789)。
文摘Cd-based Cs_(7)Cd_(3)Br_(13)perovskites,featuring both tetrahedral and octahedral polyhedral structures,have garnered significant acclaim for their efficient luminescent performance achieved through multi-exciton state regulation by doping.However,it remains controversial whether the doping sites are in the octahedra or tetrahedra of Cs_(7)Cd_(3)Br_(13).To address this,we introduced Pb^(2+)and Sb^(3+)ions and,supported by experimental and theoretical evidence,demonstrated that these ions preferentially occupy the octahedra.Among them,Pb^(2+)ions single doping achieves a near-unity photoluminescence quantum yield of 93.7%,which results in excellent X-ray scintillation performance,high light yield of 41,772 photon MeV^(-1),and a low detection limit of 29.78 nGyairs-1.Moreover,this incorporation of Pb^(2+)and Sb^(3+)enabled an exciton state regulation strategy,resulting in standard white light emission with CIE chromaticity coordinates of(0.33,0.33).Additionally,a multifaceted optical anticounterfeiting and information encryption scheme was designed based on the differences in optical properties caused by the different sensitivities of[PbBr6]4-octahedron and[SbBr6]3-octahedron to temperature and excitation wavelengths.These diverse photoluminescence characteristics provide new insights and practical demonstrations for advanced X-ray imaging,lighting,optical encryption,and anticounterfeiting technologies.
基金supported by the National Research Foundation (NRF),Prime Minister’s Office,Singapore under its NRF Fellowship (NRF2009NRF-RF001-015)Campus for Research Excellence and Technological Enterprise (CREATE)Programme-Singapore Peking University Research Centre for a Sustainable Low-Carbon Futurethe NTU-A*Star Centre of Excellence for Silicon Technologies (A*Star SERC No.:1123510003).
文摘An imine-based nitrogen-rich covalent-organic framework(COF)was successfully synthesized using two tri-angular building units under solvothermal reaction condition.The gas adsorption properties of the obtained micro-porous nitrogen-rich COF were investigated.The results indicated that the activated COF material presented good up take capabilities of CO_(2) and CH_(4) at 61.2 and 43.4 cm^(3)·g^(−1)at 1 atm and 273 K,respectively,showing its applica-tion potential in selective gas capture and separation.
基金financially supported by National Natural Science Foundation of China(grant No.22208075)Hainan Provincial Natural Science Foundation of China(grant No.522QN276)。
文摘Nucleation is a critical stage during the crystallization process,determining the attributes of the crystalline products.Due to the complicated and microscopic characteristics of the molecular assembly process,the nucleation mechanism has not yet been fully comprehended.In this study,the molecular self-assembly of 4-bromopyrazole(BMPZ)in various solvents and its relation with nucleation kinetics were investigated by the experiment and molecule simulation.Firstly,Fourier transform infrared spectroscopy,nuclear magnetic resonance spectroscopy,and mass spectroscopy were employed to explore and determine the existed forms of BMPZ molecules in solution.It was unveiled that the BMPZ molecules assembly behavior showed an individual feature.Afterward,the nucleation kinetics was determined by statistical probability distribution method,and the parameters associated with the nucleation process were derived from classical nucleation theory,further associating with the nucleation kinetics.Solution chemistry,molecule simulation,and nucleation kinetics exposed that BMPZ assembly forms could act as the growth unit of the nucleation,and nucleation kinetics was chiefly governed by the interface-transfer process.
