Because of their better chemical stability and fascinating anisotropic characteristics,Dion-Jacobson(DJ)-layered halide perovskites,which owe crystallographic two-dimensional structures,have fascinated growing attenti...Because of their better chemical stability and fascinating anisotropic characteristics,Dion-Jacobson(DJ)-layered halide perovskites,which owe crystallographic two-dimensional structures,have fascinated growing attention for solar devices.DJ-layered halide perovskites have special structural and photoelectronic features that allow the van der Waals gap to be eliminated or reduced.DJ-layered halide perovskites have improved photophysical characteristics,resulting in improved photovoltaic performance.Nevertheless,owing to the nature of the solution procedure and the fast crystal development of DJ perovskite thin layers,the precursor compositions and processing circumstances can cause a variety of defects to occur.The application of additives can impact DJ perovskite crystallization and film generation,trap passivation in the bulk and/or at the surface,interface structure,and energetic tuning.This study discusses recent developments in additive engineering for DJ multilayer halide perovskite film production.Several additive-assisted bulk and interface optimization methodologies are summarized.Lastly,an overview of research developments in additive engineering in the production of DJ-layered halide perovskite solar cells is offered.展开更多
Ga-doped Li_(7)La_(3)Zr_(2)O_(12)(Ga-LLZO)has long been considered as a promising garnet-type electrolyte candidate for all-solid-state lithium metal batteries(ASSLBs)due to its high room temperature ionic conductivit...Ga-doped Li_(7)La_(3)Zr_(2)O_(12)(Ga-LLZO)has long been considered as a promising garnet-type electrolyte candidate for all-solid-state lithium metal batteries(ASSLBs)due to its high room temperature ionic conductivity.However,the typical synthesis of Ga-LLZO is usually accompanied by the formation of undesired LiGaO_(2) impurity phase that causes severe instability of the electrolyte in contact with molten Li metal during half/full cell assembly.In this study,we show that by simply engineering the defect chemistry of Ga-LLZO,namely,the lithium deficiency level,LiGaO_(2) impurity phase is effectively inhibited in the final synthetic product.Consequently,defect chemistry engineered Ga-LLZO exhibits excellent electrochemical stability against lithium metal,while its high room temperature ionic conductivity(~1.9×10^(-3)S·cm^(-1))is well reserved.The assembled Li/Ga-LLZO/Li symmetric cell has a superior critical current density of 0.9 mA·cm^(-2),and cycles stably for 500 hours at a current density of 0.3 mA·cm^(-2).This research facilitates the potential commercial applications of high performance Ga-LLZO solid electrolytes in ASSLBs.展开更多
The interface defects between the electron transport layer(ETL)and the perovskite layer,as well as the low ultraviolet(UV)light utilization rate of the perovskite absorption layer,pose significant challenges for the c...The interface defects between the electron transport layer(ETL)and the perovskite layer,as well as the low ultraviolet(UV)light utilization rate of the perovskite absorption layer,pose significant challenges for the commercialization of perovskite solar cells(PSCs).To address this issue,this paper proposes an innovative multifunctional interface modulation strategy by introducing aggregation-induced emission(AIE)molecule 5-[4-[1,2,2-tri[4-(3,5-dicarboxyphenyl)phenyl]ethylene]phenyl]benzene-1,3-dicarboxylic acid(H_(8)ETTB)at the SnO_(2)ETL/perovskite interface.Firstly,the interaction of H_(8)ETTB with the SnO_(2)surface,facilitated by its carboxyl groups,is effective in passivating surface defects caused by noncoord inated Sn and O vacancies.This interaction enhances the conductivity of the SnO_(2)film and adjusts energy levels,leading to enhanced charge carrier transport.Simultaneously,H_(8)ETTB can passivate noncoord inated Pb^(2+)ions at the perovskite interface,promoting perovskite crystallization and reducing the interface energy barrier,resulting in a perovskite film with low defects and high crystalline quality.More importantly,the H_(8)ETTB molecule,can convert UV light into light absorbable by the perovskite,thereby reducing damage caused by UV light and improving the device's utilization of UV.Consequently,the champion PSC based on SnO_(2)-H_(8)ETTB achieves an impressing efficiency of 23.32%and significantly improved photostability compared with the control device after continuous exposure to intense UV radiation.In addition,the Cs_(0.05)(FA_(0.95)MA_(0.05))_(0.95)Pb(I_(0.95)Br_(0.05))_(3)based device can achieve maximum efficiency of 24.01%,demonstrating the effectiveness and universality of this strategy.Overall,this innovative interface bridging strategy effectively tackles interface defects and low UV light utilization in PSCs,presenting a promising approach for achieving highly efficient and stable PSCs.展开更多
CsPbI_(2)Br perovskite solar cells(PSCs)have drawn tremendous attention due to their suitable bandgap,excellent photothermal stability,and great potential as an ideal candidate for top cells in tandem solar cells.Howe...CsPbI_(2)Br perovskite solar cells(PSCs)have drawn tremendous attention due to their suitable bandgap,excellent photothermal stability,and great potential as an ideal candidate for top cells in tandem solar cells.However,the abundant defects at the buried interface and perovskite layer induce severe charge recombination,resulting in the open-circuit voltage(V_(oc))output and stability much lower than anticipated.Herein,a novel buried interface management strategy is developed to regulate interfacial carrier dynamics and CsPbI_(2)Br defects by introducing ammonium tetrafluoroborate(NH_(4)BF_(4)),thereby resulting in both high CsPbI_(2)Br crystallization and minimized interfacial energy losses.Specifically,NH_(4)^(+)ions could preferentially heal hydroxyl groups on the SnO_(2)surface and balance energy level alignment between SnO_(2)and CsPbI_(2)Br,enhancing charge transport efficiency,while BF_(4)^(-)anions as a quasi-halogen regulate crystal growth of CsPbI_(2)Br,thus reducing perovskite defects.Additionally,it is proved that eliminating hydroxyl groups at the buried interface enhances the iodide migration activation energy of CsPbI_(2)Br for strengthening the phase stability.As a result,the optimized CsPbI_(2)Br PSCs realize a remarkable efficiency of 17.09%and an ultrahigh V_(oc)output of 1.43 V,which is one of the highest values for CsPbI_(2)Br PSCs.展开更多
Although the performance of perovskite solar cells(PSCs)has been dramatically increased in recent years,stability is still the main obstacle preventing the PSCs from being commercial.PSC device instability can be caus...Although the performance of perovskite solar cells(PSCs)has been dramatically increased in recent years,stability is still the main obstacle preventing the PSCs from being commercial.PSC device instability can be caused by a variety of reasons,including ions diffusion,surface and grain boundary defects,etc.In this work,the cross-linkable tannic acid(TA)is introduced to modify perovskite film through post-treatment method.The numerous organic functional groups(–OH and C=O)in TA can interact with the uncoordinated Pb^(2+)and I^(-)ions in perovskite,thus passivating defects and inhibiting ions diffusion.In addition,the formed TA network can absorb a small amount of the residual moisture inside the device to protect the perovskite layer.Furthermore,TA modification regulates the energy level of perovskite,and reduces interfacial charge recombination.Ultimately,following TA treatment,the device efficiency is increased significantly from 21.31%to 23.11%,with a decreased hysteresis effect.Notably,the treated device shows excellent air,thermal,and operational stability.In light of this,the readily available,inexpensive TA has the potential to operate as a multipurpose interfacial modifier to increase device efficiency while also enhancing device stability.展开更多
Two-dimensional(2D)membrane-based ion separation technology has been increasingly explored to address the problem of lithium resource shortage,yet it remains a sound challenge to design 2D membranes of high selectivit...Two-dimensional(2D)membrane-based ion separation technology has been increasingly explored to address the problem of lithium resource shortage,yet it remains a sound challenge to design 2D membranes of high selectivity and permeability for ion separation applications.Zeolitic imidazolate framework functionalized modified layered double hydroxide(ZIF-8@MLDH)composite membranes with high lithium-ion(Li^(+)) permeability and excellent operational stability were obtained in this work by in situ depositing functional ZIF-8 nanoparticles into the nanopores acting as framework defects in MLDH membranes.The defect-rich framework amplified the permeability of Li^(+),and the site-selective growth of ZIF-8 in the framework defects bettered its selectivity.Specifically speaking,the ZIF-8@MLDH membranes featured a high permeation rate of Li^(+) up to 1.73 mol m^(−2) h^(−1) and a desirable selectiv-ity of Li^(+)/Mg^(2+) up to 31.9.Simulations supported that the simultaneously enhanced selectivity and permeability of Li+are attributed to changes in the type of mass transfer channels and the difference in the dehydration capacity of hydrated metal cations when they pass through nanochannels of ZIF-8.This study will inspire the ongoing research of high-performance 2D membranes through the engineering of defects.展开更多
基金Min Liu thanks the CSC for funding his PhD scholarship(grant number 202008120110)The ANR agency is acknowledged for financial support via the ChemSta project ANR-21-CE05-0022.
文摘Because of their better chemical stability and fascinating anisotropic characteristics,Dion-Jacobson(DJ)-layered halide perovskites,which owe crystallographic two-dimensional structures,have fascinated growing attention for solar devices.DJ-layered halide perovskites have special structural and photoelectronic features that allow the van der Waals gap to be eliminated or reduced.DJ-layered halide perovskites have improved photophysical characteristics,resulting in improved photovoltaic performance.Nevertheless,owing to the nature of the solution procedure and the fast crystal development of DJ perovskite thin layers,the precursor compositions and processing circumstances can cause a variety of defects to occur.The application of additives can impact DJ perovskite crystallization and film generation,trap passivation in the bulk and/or at the surface,interface structure,and energetic tuning.This study discusses recent developments in additive engineering for DJ multilayer halide perovskite film production.Several additive-assisted bulk and interface optimization methodologies are summarized.Lastly,an overview of research developments in additive engineering in the production of DJ-layered halide perovskite solar cells is offered.
基金financially supported by the National Natural Science Foundation of China (Grant No.52171221)the National Key Research and Development Program of China (Grant No.2019YFA0704900)。
文摘Ga-doped Li_(7)La_(3)Zr_(2)O_(12)(Ga-LLZO)has long been considered as a promising garnet-type electrolyte candidate for all-solid-state lithium metal batteries(ASSLBs)due to its high room temperature ionic conductivity.However,the typical synthesis of Ga-LLZO is usually accompanied by the formation of undesired LiGaO_(2) impurity phase that causes severe instability of the electrolyte in contact with molten Li metal during half/full cell assembly.In this study,we show that by simply engineering the defect chemistry of Ga-LLZO,namely,the lithium deficiency level,LiGaO_(2) impurity phase is effectively inhibited in the final synthetic product.Consequently,defect chemistry engineered Ga-LLZO exhibits excellent electrochemical stability against lithium metal,while its high room temperature ionic conductivity(~1.9×10^(-3)S·cm^(-1))is well reserved.The assembled Li/Ga-LLZO/Li symmetric cell has a superior critical current density of 0.9 mA·cm^(-2),and cycles stably for 500 hours at a current density of 0.3 mA·cm^(-2).This research facilitates the potential commercial applications of high performance Ga-LLZO solid electrolytes in ASSLBs.
基金finically supported by the National Natural Science Foundation of China(62350054,12374379,12174152,12304462)the Foundation of National Key Laboratory(***202302011)。
文摘The interface defects between the electron transport layer(ETL)and the perovskite layer,as well as the low ultraviolet(UV)light utilization rate of the perovskite absorption layer,pose significant challenges for the commercialization of perovskite solar cells(PSCs).To address this issue,this paper proposes an innovative multifunctional interface modulation strategy by introducing aggregation-induced emission(AIE)molecule 5-[4-[1,2,2-tri[4-(3,5-dicarboxyphenyl)phenyl]ethylene]phenyl]benzene-1,3-dicarboxylic acid(H_(8)ETTB)at the SnO_(2)ETL/perovskite interface.Firstly,the interaction of H_(8)ETTB with the SnO_(2)surface,facilitated by its carboxyl groups,is effective in passivating surface defects caused by noncoord inated Sn and O vacancies.This interaction enhances the conductivity of the SnO_(2)film and adjusts energy levels,leading to enhanced charge carrier transport.Simultaneously,H_(8)ETTB can passivate noncoord inated Pb^(2+)ions at the perovskite interface,promoting perovskite crystallization and reducing the interface energy barrier,resulting in a perovskite film with low defects and high crystalline quality.More importantly,the H_(8)ETTB molecule,can convert UV light into light absorbable by the perovskite,thereby reducing damage caused by UV light and improving the device's utilization of UV.Consequently,the champion PSC based on SnO_(2)-H_(8)ETTB achieves an impressing efficiency of 23.32%and significantly improved photostability compared with the control device after continuous exposure to intense UV radiation.In addition,the Cs_(0.05)(FA_(0.95)MA_(0.05))_(0.95)Pb(I_(0.95)Br_(0.05))_(3)based device can achieve maximum efficiency of 24.01%,demonstrating the effectiveness and universality of this strategy.Overall,this innovative interface bridging strategy effectively tackles interface defects and low UV light utilization in PSCs,presenting a promising approach for achieving highly efficient and stable PSCs.
基金supported by the National Natural Science Foundation of China(22379010,22109166,22309191)Chinese Academy of Sciences。
文摘CsPbI_(2)Br perovskite solar cells(PSCs)have drawn tremendous attention due to their suitable bandgap,excellent photothermal stability,and great potential as an ideal candidate for top cells in tandem solar cells.However,the abundant defects at the buried interface and perovskite layer induce severe charge recombination,resulting in the open-circuit voltage(V_(oc))output and stability much lower than anticipated.Herein,a novel buried interface management strategy is developed to regulate interfacial carrier dynamics and CsPbI_(2)Br defects by introducing ammonium tetrafluoroborate(NH_(4)BF_(4)),thereby resulting in both high CsPbI_(2)Br crystallization and minimized interfacial energy losses.Specifically,NH_(4)^(+)ions could preferentially heal hydroxyl groups on the SnO_(2)surface and balance energy level alignment between SnO_(2)and CsPbI_(2)Br,enhancing charge transport efficiency,while BF_(4)^(-)anions as a quasi-halogen regulate crystal growth of CsPbI_(2)Br,thus reducing perovskite defects.Additionally,it is proved that eliminating hydroxyl groups at the buried interface enhances the iodide migration activation energy of CsPbI_(2)Br for strengthening the phase stability.As a result,the optimized CsPbI_(2)Br PSCs realize a remarkable efficiency of 17.09%and an ultrahigh V_(oc)output of 1.43 V,which is one of the highest values for CsPbI_(2)Br PSCs.
基金supported by the General Program of Chongqing Natural Science Foundation(CSTB2022NSCQMSX1227 and CSTB2022NSCQ-MSX0459)the supports from the Fundamental Research Funds for the Central Universities(SWU-XDJH202314)。
文摘Although the performance of perovskite solar cells(PSCs)has been dramatically increased in recent years,stability is still the main obstacle preventing the PSCs from being commercial.PSC device instability can be caused by a variety of reasons,including ions diffusion,surface and grain boundary defects,etc.In this work,the cross-linkable tannic acid(TA)is introduced to modify perovskite film through post-treatment method.The numerous organic functional groups(–OH and C=O)in TA can interact with the uncoordinated Pb^(2+)and I^(-)ions in perovskite,thus passivating defects and inhibiting ions diffusion.In addition,the formed TA network can absorb a small amount of the residual moisture inside the device to protect the perovskite layer.Furthermore,TA modification regulates the energy level of perovskite,and reduces interfacial charge recombination.Ultimately,following TA treatment,the device efficiency is increased significantly from 21.31%to 23.11%,with a decreased hysteresis effect.Notably,the treated device shows excellent air,thermal,and operational stability.In light of this,the readily available,inexpensive TA has the potential to operate as a multipurpose interfacial modifier to increase device efficiency while also enhancing device stability.
基金The authors gratefully acknowledge the funding from the Natural Science Foundation of China(22125801,22178008)the Importation and Development of High-Caliber Talents Project of Beijing Municipal Institutions(CIT&TCD201904014)+1 种基金Jiayin Yuan is grateful for financial support from Swedish Research Council Grant 2018-05351the Wallenberg Academy Fellow program(Grant KAW 2017.0166)from the Knut&Alice Wallenberg Foundation in Sweden.
文摘Two-dimensional(2D)membrane-based ion separation technology has been increasingly explored to address the problem of lithium resource shortage,yet it remains a sound challenge to design 2D membranes of high selectivity and permeability for ion separation applications.Zeolitic imidazolate framework functionalized modified layered double hydroxide(ZIF-8@MLDH)composite membranes with high lithium-ion(Li^(+)) permeability and excellent operational stability were obtained in this work by in situ depositing functional ZIF-8 nanoparticles into the nanopores acting as framework defects in MLDH membranes.The defect-rich framework amplified the permeability of Li^(+),and the site-selective growth of ZIF-8 in the framework defects bettered its selectivity.Specifically speaking,the ZIF-8@MLDH membranes featured a high permeation rate of Li^(+) up to 1.73 mol m^(−2) h^(−1) and a desirable selectiv-ity of Li^(+)/Mg^(2+) up to 31.9.Simulations supported that the simultaneously enhanced selectivity and permeability of Li+are attributed to changes in the type of mass transfer channels and the difference in the dehydration capacity of hydrated metal cations when they pass through nanochannels of ZIF-8.This study will inspire the ongoing research of high-performance 2D membranes through the engineering of defects.
