To date, the instability of organometal halide perovskite solar cells(PSCs) has become the focus issue that limits the development and long-term application of PSCs. Both the ultraviolet(UV) rays in sunlight and m...To date, the instability of organometal halide perovskite solar cells(PSCs) has become the focus issue that limits the development and long-term application of PSCs. Both the ultraviolet(UV) rays in sunlight and moisture in air can significantly accelerate the disintegration of the perovskite. Here, we introduced a Zn Se quantum dots layer as downshifting materials, which was spin-coated onto the backside of PSCs.This layer converted the UV rays into visible light to prevent the destruction of PSCs as well as increase the light harvesting of the perovskite layer. Under the UV irradiation in the moisture ambient(40%), the destruction speed of the unencapsulated perovskite films were also delayed evidently. In addition, the power conversion efficiency(PCE) of the PSCs was increased from 16.6% to 17.3% due to the increase of the visible light absorbance of the perovskite.展开更多
Lead halide perovskite quantum dots(PQDs) have recently emerged as promising light absorbers for photovoltaic application due to their extraordinary optoelectronic properties. Surface ligands are of utmost importance ...Lead halide perovskite quantum dots(PQDs) have recently emerged as promising light absorbers for photovoltaic application due to their extraordinary optoelectronic properties. Surface ligands are of utmost importance for the colloidal stability and property tuning of PQDs, while their highly dynamic binding nature not only impedes further efficiency improvement of PQD-based solar cells but also induces intrinsic instability. Tremendous efforts have been made in ligand engineering with good hopes to solve such challenging issues in the past few years. In this review, we first present a fundamental understanding of the role of surface ligands in PQDs, followed by a brief discussion and classification of various ligands that have the potential for improving the electronic coupling and stability of PQD solids. We then provide a critical overview of recent advances in ligand engineering including the strategies of in-situ ligand engineering, postsynthesis/-deposition ligand-exchange, and interfacial engineering, and discuss their impacts on changing the efficiency and stability of perovskite QD solar cells(QDSCs). Finally, we give our perspectives on the future directions of ligand engineering towards more efficient and stable perovskite QDSCs.展开更多
Perovskite quantum dots(PQDs)have been considered promising and effective photovoltaic absorber due to their superior optoelectronic properties and inherent material merits combining perovskites and QDs.However,they e...Perovskite quantum dots(PQDs)have been considered promising and effective photovoltaic absorber due to their superior optoelectronic properties and inherent material merits combining perovskites and QDs.However,they exhibit low moisture stability at room humidity(20-30%)owing to many surface defect sites generated by inefficient ligand exchange process.These surface traps must be re-passivated to improve both charge transport ability and moisture stability.To address this issue,PQD-organic semiconductor hybrid solar cells with suitable electrical properties and functional groups might dramatically improve the charge extraction and defect passivation.Conventional organic semiconductors are typically low-dimensional(1D and 2D)and prone to excessive self-aggregation,which limits chemical interaction with PQDs.In this work,we designed a new 3D star-shaped semiconducting material(Star-TrCN)to enhance the compatibility with PQDs.The robust bonding with Star-TrCN and PQDs is demonstrated by theoretical modeling and experimental validation.The Star-TrCN-PQD hybrid films show improved cubic-phase stability of CsPbI_(3)-PQDs via reduced surface trap states and suppressed moisture penetration.As a result,the resultant devices not only achieve remarkable device stability over 1000 h at 20-30%relative humidity,but also boost power conversion efficiency up to 16.0%via forming a cascade energy band structure.展开更多
All-inorganic cesium lead bromide(CsPbBr_(3))perovskite solar cells have been attracting growing interest due to superior performance stability and low cost.However,low light absorbance and large charge recombination ...All-inorganic cesium lead bromide(CsPbBr_(3))perovskite solar cells have been attracting growing interest due to superior performance stability and low cost.However,low light absorbance and large charge recombination at TiO_(2)/CsPbBr_(3)interface or within CsPbBr_(3)film still prevent further performance improvement.Herein,we report devices with high power conversion efficiency(9.16%)by introducing graphene oxide quantum dots(GOQDs)between TiO_(2)and perovskite layers.The recombination of interfacial radiation can be effectively restrained due to enhanced charge transfer capability.GOQDs with C-rich active sites can involve in crystallization and fill within the CsPbBr_(3)perovskite film as functional semiconductor additives.This work provides a promising strategy to optimize the crystallization process and boost charge extraction at the surface/interface optoelectronic properties of perovskites for high efficient and low-cost solar cells.展开更多
Inorganic halide perovskites CsPb X_3(X = I, Br) have attracted tremendous attention in solar cell applications. However, the bulk form of the cubic phase CsPb X_3, which offers moderate direct bandgaps, is metastable...Inorganic halide perovskites CsPb X_3(X = I, Br) have attracted tremendous attention in solar cell applications. However, the bulk form of the cubic phase CsPb X_3, which offers moderate direct bandgaps, is metastable at room temperature and tends to transform into a tetragonal or orthorhombic phase. Here, our density functional theory calculation results found that the surface energies of the cubic phase are smaller than those of the orthorhombic phase, although the bulk counterpart of the cubic phase is less stable than that of the orthorhombic phase. These results suggest a surface stabilization strategy to maintain the stability of the cubic phase at room temperature that an enlarged portion of surfaces shall change the relative stability of the two phases in nanostructured CsPb X_3. This strategy, which may potentially solve the long-standing stability issue of cubic CsPb X_3, was demonstrated to be feasible by our calculations in zero-, one-, and two-dimensional nanostructures. In particular, confined sizes from few to tens of nanometers could keep the cubic phase as the most thermally favored form at room temperature. Our predicted values in particular cases, such as the zero-dimensional form of CsPbI_3,are highly consistent with experimental values, suggesting that our model is reasonable and our results are reliable. These predicted critical sizes give the upper and lower limits of the confined sizes, which may guide experimentalists to synthesize these nanostructures and promote likely practical applications such as solar cells and flexible displays using CsPb X_3 nanostructures.展开更多
基金supported by the National Science Foundation of China (51774034, 51772026, 51611130063)the Fundamental Research Funds for the Central Universities (FRF-BD-16-012A)111 Project (No. B17003)
文摘To date, the instability of organometal halide perovskite solar cells(PSCs) has become the focus issue that limits the development and long-term application of PSCs. Both the ultraviolet(UV) rays in sunlight and moisture in air can significantly accelerate the disintegration of the perovskite. Here, we introduced a Zn Se quantum dots layer as downshifting materials, which was spin-coated onto the backside of PSCs.This layer converted the UV rays into visible light to prevent the destruction of PSCs as well as increase the light harvesting of the perovskite layer. Under the UV irradiation in the moisture ambient(40%), the destruction speed of the unencapsulated perovskite films were also delayed evidently. In addition, the power conversion efficiency(PCE) of the PSCs was increased from 16.6% to 17.3% due to the increase of the visible light absorbance of the perovskite.
基金the financial support from the Australian Research Council (ARC) Laureate Fellowship (FL190100139)the ARC Discovery Project (DP200101900)+3 种基金the CRC-P programsthe funding support from the ARC through Discovery Early Career Researcher Award Fellowship (DE190101351)the Discovery Project (DP190102507)the financial support from University of Queensland Research Training Scholarship。
文摘Lead halide perovskite quantum dots(PQDs) have recently emerged as promising light absorbers for photovoltaic application due to their extraordinary optoelectronic properties. Surface ligands are of utmost importance for the colloidal stability and property tuning of PQDs, while their highly dynamic binding nature not only impedes further efficiency improvement of PQD-based solar cells but also induces intrinsic instability. Tremendous efforts have been made in ligand engineering with good hopes to solve such challenging issues in the past few years. In this review, we first present a fundamental understanding of the role of surface ligands in PQDs, followed by a brief discussion and classification of various ligands that have the potential for improving the electronic coupling and stability of PQD solids. We then provide a critical overview of recent advances in ligand engineering including the strategies of in-situ ligand engineering, postsynthesis/-deposition ligand-exchange, and interfacial engineering, and discuss their impacts on changing the efficiency and stability of perovskite QD solar cells(QDSCs). Finally, we give our perspectives on the future directions of ligand engineering towards more efficient and stable perovskite QDSCs.
基金This work was supported by National Research Foundation of Korea(NRF)grants funded by Ministry of Science and ICT(MSIT)(Nos.2021R1A2C3004420,2022M3J1A1085282,2020R1C1C1012256 and 2020R1C1C1003214)the NRF of Korea grant funded by the Korean Government(NRF-2019-Global Ph.D.Fellowship Program.
文摘Perovskite quantum dots(PQDs)have been considered promising and effective photovoltaic absorber due to their superior optoelectronic properties and inherent material merits combining perovskites and QDs.However,they exhibit low moisture stability at room humidity(20-30%)owing to many surface defect sites generated by inefficient ligand exchange process.These surface traps must be re-passivated to improve both charge transport ability and moisture stability.To address this issue,PQD-organic semiconductor hybrid solar cells with suitable electrical properties and functional groups might dramatically improve the charge extraction and defect passivation.Conventional organic semiconductors are typically low-dimensional(1D and 2D)and prone to excessive self-aggregation,which limits chemical interaction with PQDs.In this work,we designed a new 3D star-shaped semiconducting material(Star-TrCN)to enhance the compatibility with PQDs.The robust bonding with Star-TrCN and PQDs is demonstrated by theoretical modeling and experimental validation.The Star-TrCN-PQD hybrid films show improved cubic-phase stability of CsPbI_(3)-PQDs via reduced surface trap states and suppressed moisture penetration.As a result,the resultant devices not only achieve remarkable device stability over 1000 h at 20-30%relative humidity,but also boost power conversion efficiency up to 16.0%via forming a cascade energy band structure.
基金supported by the National Natural Science Foundation of China(Grant Nos.21776147,21905153,61604086)the Qingdao Municipal Science and Technology Bureau(Grant No.19-6-1-91-nsh)A Project of Shandong Province Higher Educational Science and Technology Program(Grant No.J17KA013).
文摘All-inorganic cesium lead bromide(CsPbBr_(3))perovskite solar cells have been attracting growing interest due to superior performance stability and low cost.However,low light absorbance and large charge recombination at TiO_(2)/CsPbBr_(3)interface or within CsPbBr_(3)film still prevent further performance improvement.Herein,we report devices with high power conversion efficiency(9.16%)by introducing graphene oxide quantum dots(GOQDs)between TiO_(2)and perovskite layers.The recombination of interfacial radiation can be effectively restrained due to enhanced charge transfer capability.GOQDs with C-rich active sites can involve in crystallization and fill within the CsPbBr_(3)perovskite film as functional semiconductor additives.This work provides a promising strategy to optimize the crystallization process and boost charge extraction at the surface/interface optoelectronic properties of perovskites for high efficient and low-cost solar cells.
基金Project supported by the National Natural Science Foundation of China(Grant Nos.91433103,11622437,and 61674171)the Fundamental Research Funds for the Central Universities of China+1 种基金the Research Funds of Renmin University of China(Grant Nos.16XNLQ01 and 19XNH065)the Strategic Priority Research Program of Chinese Academy of Sciences(Grant No.XDB30000000)
文摘Inorganic halide perovskites CsPb X_3(X = I, Br) have attracted tremendous attention in solar cell applications. However, the bulk form of the cubic phase CsPb X_3, which offers moderate direct bandgaps, is metastable at room temperature and tends to transform into a tetragonal or orthorhombic phase. Here, our density functional theory calculation results found that the surface energies of the cubic phase are smaller than those of the orthorhombic phase, although the bulk counterpart of the cubic phase is less stable than that of the orthorhombic phase. These results suggest a surface stabilization strategy to maintain the stability of the cubic phase at room temperature that an enlarged portion of surfaces shall change the relative stability of the two phases in nanostructured CsPb X_3. This strategy, which may potentially solve the long-standing stability issue of cubic CsPb X_3, was demonstrated to be feasible by our calculations in zero-, one-, and two-dimensional nanostructures. In particular, confined sizes from few to tens of nanometers could keep the cubic phase as the most thermally favored form at room temperature. Our predicted values in particular cases, such as the zero-dimensional form of CsPbI_3,are highly consistent with experimental values, suggesting that our model is reasonable and our results are reliable. These predicted critical sizes give the upper and lower limits of the confined sizes, which may guide experimentalists to synthesize these nanostructures and promote likely practical applications such as solar cells and flexible displays using CsPb X_3 nanostructures.