In backlighting systems for liquid crystal displays,conventional red,green,and blue(RGB)light sources that lack polarization properties can result in a significant optical loss of up to 50%when passing through a polar...In backlighting systems for liquid crystal displays,conventional red,green,and blue(RGB)light sources that lack polarization properties can result in a significant optical loss of up to 50%when passing through a polarizer.To address this inefficiency and optimize energy utilization,this study presents a high-performance device designed for RGB polarized emissions.The device employs an array of semipolar blueμLEDs with inherent polarization capabilities,coupled with mechanically stretched films of green-emitting CsPbBr3 nanorods and red-emitting CsPbI3-Cs4PbI6 hybrid nanocrystals.The CsPbBr3 nanorods in the polymer film offer intrinsic polarization emission,while the aligned-wire structures formed by the stable CsPbI3-Cs4PbI6 hybrid nanocrystals contribute to substantial anisotropic emissions,due to their high dielectric constant.The resulting device achieved RGB polarization degrees of 0.26,0.48,and 0.38,respectively,and exhibited a broad color gamut,reaching 137.2%of the NTSC standard and 102.5%of the Rec.2020 standard.When compared to a device utilizing c-plane LEDs for excitation,the current approach increased the intensity of light transmitted through the polarizer by 73.6%.This novel fabrication approach for polarized devices containing RGB components holds considerable promise for advancing next-generation display technologies.展开更多
The incorporation of partial A-site substitution in perovskite oxides represents a promising strategy for precisely controlling the electronic configuration and enhancing its intrinsic catalytic activity.Conventional ...The incorporation of partial A-site substitution in perovskite oxides represents a promising strategy for precisely controlling the electronic configuration and enhancing its intrinsic catalytic activity.Conventional methods for A-site substitution typically involve prolonged high-temperature processes.While these processes promote the development of unique nanostructures with highly exposed active sites,they often result in the uncontrolled configuration of introduced elements.Herein,we present a novel approach for synthesizing two-dimensional(2D)porous GdFeO_(3) perovskite with A-site strontium(Sr)substitution utilizing microwave shock method.This technique enables precise control of the Sr content and simultaneous construction of 2D porous structures in one step,capitalizing on the advantages of rapid heating and cooling(temperature~1100 K,rate~70 K s^(-1)).The active sites of this oxygen-rich defect structure can be clearly revealed through the simulation of the electronic configuration and the comprehensive analysis of the crystal structure.For electrocatalytic oxygen evolution reaction application,the synthesized 2D porous Gd_(0.8)Sr_(0.2)FeO_(3) electrocatalyst exhibits an exceptional overpotential of 294 mV at a current density of 10 mA cm^(-2)and a small Tafel slope of 55.85 mV dec^(-1)in alkaline electrolytes.This study offers a fresh perspective on designing crystal configurations and the construction of nanostructures in perovskite.展开更多
Wide bandgap perovskite solar cells(PSCs)have attracted significant attention because they can be applied to the top cells of tandem solar cells.However,high open-circuit voltage(V_(OC))deficit(>0.4 V)result from p...Wide bandgap perovskite solar cells(PSCs)have attracted significant attention because they can be applied to the top cells of tandem solar cells.However,high open-circuit voltage(V_(OC))deficit(>0.4 V)result from poor crystallization and high non-radiative recombination losses become a serious limitation in the pursuit of high performance.Here,the relevance between different Pbl_(2)proportions and performance parameters are revealed through analysis of surface morphology,residual stress,and photostability.The increase of Pbl_(2)proportion promotes crystal growth and reduces the work function of the perovskite film surface and promotes the energy level alignment with the carrier transport layer,which decreased the V_(OC)deficit.However,residual PbI_(2)exacerbated the stress level of perovskite film,and the resulting lattice disorder deteriorated the photostability of the device.Ultimately,after the synergistic passivation of residual PbI_(2)and PEAI,the V_(OC)achieves 1.266 V and V_(OC)deficit is less than 0.4 V,the record value in wide bandgap PSCs.展开更多
NiO_(x)as a hole transport material for inverted perovskite solar cells has received great attention owing to its high transparency,low fabrication temperature,and superior stability.However,the mismatched energy leve...NiO_(x)as a hole transport material for inverted perovskite solar cells has received great attention owing to its high transparency,low fabrication temperature,and superior stability.However,the mismatched energy levels and possible redox reactions at the NiO_(x)/perovskite interface severely limit the performance of NiO_(x) based inverted perovskite solar cells.Herein,we introduce a p-type self-assembled monolayer between NiO_(x)and perovskite layers to modify the interface and block the undesirable redox reaction between perovskite and NiO_(x)The selfassembled monolayer molecules all contain phosphoric acid function groups,which can be anchored onto the NiOr surface and passivate the surface defect.Moreover,the introduction of self-assembled monolayers can regulate the energy level structure of NiO_(x),reduce the interfacial band energy offset,and hence promote the hole transport from perovskite to NiO_(x)layer.Consequently,the device performance is significantly enhanced in terms of both power conversion efficiency and stability.展开更多
Developing efficient and stable cathodes for low-temperature solid oxide fuel cells(LT-SOFCs) is of great importance for the practical commercialization.Herein,we propose a series of Sm-modified Bi_(0.7-x)Sm_xSr_(0.3)...Developing efficient and stable cathodes for low-temperature solid oxide fuel cells(LT-SOFCs) is of great importance for the practical commercialization.Herein,we propose a series of Sm-modified Bi_(0.7-x)Sm_xSr_(0.3)FeO_(3-δ) perovskites as highly-active catalysts for LT-SOFCs.Sm doping can significantly enhance the electrocata lytic activity and chemical stability of cathode.At 600℃,Bi_(0.675)Sm_(0.025)Sr_(0.3)FeO_(3-δ)(BSSF25) cathode has been found to be the optimum composition with a polarization resistance of 0.098 Ω cm^2,which is only around 22.8% of Bi_(0.7)Sr_(0.3)FeO_(3-δ)(BSF).A full cell utilizing BSSF25 displays an exceptional output density of 790 mW cm^(-2),which can operate continuously over100 h without obvious degradation.The remarkable electrochemical performance observed can be attributed to the improved O_(2) transport kinetics,superior surface oxygen adsorption capacity,as well as O_(2)p band centers in close proximity to the Fermi level.Moreover,larger average bonding energy(ABE) and the presence of highly acidic Bi,Sm,and Fe ions restrict the adsorption of CO_(2) on the cathode surface,resulting in excellent CO_(2) resistivity.This work provides valuable guidance for systematic design of efficient and durable catalysts for LT-SOFCs.展开更多
The use of low-dimensional(LD)perovskite materials is crucial for achieving high-performance perovskite solar cells(PSCs).However,LD perovskite films fabricated by conventional approaches give rise to full coverage of...The use of low-dimensional(LD)perovskite materials is crucial for achieving high-performance perovskite solar cells(PSCs).However,LD perovskite films fabricated by conventional approaches give rise to full coverage of the underlying 3D perovskite films,which inevitably hinders the transport of charge carriers at the interface of PSCs.Here,we designed and fabricated LD perovskite structure that forms net-like morphology on top of the underlying three-dimensional(3D)perovskite bulk film.The net-like LD perovskite not only reduced the surface defects of 3D perovskite film,but also provided channels for the vertical transport of charge carriers,effectively enhancing the interfacial charge transfer at the LD/3D hetero-interface.The net-like morphological design comprising LD perovskite effectively resolves the contradiction between interfacial defect passivation and carrier extraction across the hetero-interfaces.Furthermore,the net-like LD perovskite morphology can enhance the stability of the underlying 3D perovskite film,which is attributed to the hydrophobic nature of LD perovskite.As a result,the net-like LD perovskite film morphology assists PSCs in achieving an excellent power conversion efficiency of up to 24.6%with over 1000 h long-term operational stability.展开更多
Solution processability significantly advances the development of highly-efficient perovskite solar cells.However,the precursor solution tends to undergo irreversible degradation reactions,impairing the device perform...Solution processability significantly advances the development of highly-efficient perovskite solar cells.However,the precursor solution tends to undergo irreversible degradation reactions,impairing the device performance and reproducibility.Here,we utilize a reductive natural amino acid,Nacetylcysteine(NALC),to stabilize the precursor solution for printable carbon-based hole-conductorfree mesoscopic perovskite solar cells.We find that I_(2) can be generated in the aged solution containing methylammonium iodide(MI) in an inert atmosphere and speed up the MA-FA^(+)(formamidinium) reaction which produces large-size cations and hinders the formation of perovskite phase.NALC effectively stabilizes the precursor via its sulfhydryl group which reduces I_(2) back to I^(-)and provides H^(+).The NALC-stabilized precursor which is aged for 1440 h leads to devices with a power conversion efficiency equivalent to 98% of that for devices prepared with the fresh precursor.Furthermore,NALC improves the device power conversion efficiency from 16.16% to 18.41% along with enhanced stability under atmospheric conditions by modifying grain boundaries in perovskite films and reducing associated defects.展开更多
Two-dimensional Ruddlesden-Popper(2DRP)perovskite exhibits excellent stability in perovskite solar cells(PSCs)due to introducing hydrophobic long-chain organic spacers.However,the poor charge transporting property of ...Two-dimensional Ruddlesden-Popper(2DRP)perovskite exhibits excellent stability in perovskite solar cells(PSCs)due to introducing hydrophobic long-chain organic spacers.However,the poor charge transporting property of bulky organic cation spacers limits the performance of 2DRP PSCs.Inspired by the Asite cation alloying strategy in 3D perovskites,2DRP perovskites with a binary spacer can promote charge transporting compared to the unary spacer counterparts.Herein,the superior MA-based 2DRP perovskite films with a binary spacer,including 3-guanidinopropanoic acid(GPA)and 4-fluorophenethylamine(FPEA)are realized.These films(GPA_(0.85)FPEA_(0.15))_(2)MA_(4)Pb_5I_(16)show good morphology,large grain size,decreased trap state density,and preferential orientation of the as-prepared film.Accordingly,the present 2DRP-based PSC with the binary spacer achieves a remarkable efficiency of 18.37%with a V_(OC)of1.15 V,a J_(SC)of 20.13 mA cm^(-2),and an FF of 79.23%.To our knowledge,the PCE value should be the highest for binary spacer MA-based 2DRP(n≤5)PSCs to date.Importantly,owing to the hydrophobic fluorine group of FPEA and the enhanced interlayer interaction by FPEA,the unencapsulated 2DRP PSCs based on binary spacers exhibit much excellent humidity stability and thermal stability than the unary spacer counterparts.展开更多
A considerable efficiency gap exists between large-area perovskite solar modules and small-area perovskite solar cells.The control of forming uniform and large-area film and perovskite crystallization is still the mai...A considerable efficiency gap exists between large-area perovskite solar modules and small-area perovskite solar cells.The control of forming uniform and large-area film and perovskite crystallization is still the main obstacle restricting the efficiency of PSMs.In this work,we adopted a solid-liquid two-step film formation technique,which involved the evaporation of a lead iodide film and blade coating of an organic ammonium halide solution to prepare perovskite films.This method possesses the advantages of integrating vapor deposition and solution methods,which could apply to substrates with different roughness and avoid using toxic solvents to achieve a more uniform,large-area perovskite film.Furthermore,modification of the NiO_(x)/perovskite buried interface and introduction of Urea additives were utilized to reduce interface recombination and regulate perovskite crystallization.As a result,a large-area perovskite film possessing larger grains,fewer pinholes,and reduced defects could be achieved.The inverted PSM with an active area of 61.56 cm^(2)(10×10 cm^(2)substrate)achieved a champion power conversion efficiency of 20.56%and significantly improved stability.This method suggests an innovative approach to resolving the uniformity issue associated with large-area film fabrication.展开更多
The successful utilization of an eco-friendly and biocompatible parylene-C substrate for high-performance solution-processed double-walled carbon nanotube(CNT)electrode-based perovskite solar cells(PSCs)was demonstrat...The successful utilization of an eco-friendly and biocompatible parylene-C substrate for high-performance solution-processed double-walled carbon nanotube(CNT)electrode-based perovskite solar cells(PSCs)was demonstrated.Through the use of a novel inversion transfer technique,vertical separation of the binders from the CNTs was induced,rendering a stronger p-doping effect and thereby a higher conductivity of the CNTs.The resulting foldable devices exhibited a power conversion efficiency of 18.11%,which is the highest reported among CNT transparent electrode-based PSCs to date,and withstood more than 10,000 folding cycles at a radius of 0.5 mm,demonstrating unprecedented mechanical stability.Furthermore,solar modules were fabricated using entirely laser scribing processes to assess the potential of the solution-processable nanocarbon electrode.Notably,this is the only one to be processed entirely by the laser scribing process and to be biocompatible as well as eco-friendly among the previously reported nonindium tin oxide-based perovskite solar modules.展开更多
Tin-based perovskite solar cells(TPSCs)have received great attention due to their eco-friendly properties and high theoretical efficiencies.However,the fast crystallization feature of tin-based perovskites leads to po...Tin-based perovskite solar cells(TPSCs)have received great attention due to their eco-friendly properties and high theoretical efficiencies.However,the fast crystallization feature of tin-based perovskites leads to poor film quality and limits the corresponding device performance.Herein,a chlorofullerene,C_(60)Cl_(6),with six chlorine attached to the C_(60)cage,is applied to modulate the crystallization process and passivate grain boundary defects of the perovskite film.The chemical interactions between C_(60)Cl_(6)and perovskite components retard the transforming process of precursors to perovskite crystals and obtain a high-quality tin-based perovskite film.It is also revealed that the C_(60)Cl_(6)located at the surfaces and grain boundaries can not only passivate the defects but also offer a role in suturing grain boundaries to suppress the detrimental effects of water and oxygen on perovskite films,especially the oxidation of Sn^(2+)to Sn^(4+).As a result,the C_(60)Cl_(6)-based device yields a remarkably improved device efficiency from 10.03%to 13.30%with enhanced stability.This work provides a new strategy to regulate the film quality and stability of TPSCs using functional fullerene materials.展开更多
The Cs_(2)NaInCl_(6) double perovskite is one of the most promising lead-free perovskites due to its exceptional stability and straightforward synthesis.However,it faces challenges related to inefficient photoluminesc...The Cs_(2)NaInCl_(6) double perovskite is one of the most promising lead-free perovskites due to its exceptional stability and straightforward synthesis.However,it faces challenges related to inefficient photoluminescence.Doping and high pressure are employed to tailor the optical properties of Cs_(2)NaInCl_(6).Herein,Sb^(3+)doped Cs_(2)NaInCl_(6)(Sb^(3+):Cs_(2)NaInCl_(6)) was synthesized and it exhibits blue emission with a photoluminescence quantum yield of up to 37.3%.Further,by employing pressure tuning,a blue stable emission under a very wide range from 2.7 GPa to 9.8 GPa is realized in Sb^(3+):Cs_(2)NaInCl_(6).Subsequently,the emission intensity of Sb^(3+):Cs_(2)NaInCl_(6) experiences a significant increase(3.3 times)at 19.0 GPa.It is revealed that the pressure-induced distinct emissions can be attributed to the carrier self-trapping and detrapping between Cs_(2)NaInCl_(6) and Sb^(3+).Notably,the lattice compression in the cubic phase inevitably modifies the band gap of Sb^(3+):Cs_(2)NaInCl_(6).Our findings provide valuable insights into effects of the high pressure in further boosting unique emission characteristics but also offer promising opportunities for development of doped double perovskites with enhanced optical functionalities.展开更多
Near-infrared(NIR)transparent inverted all-inorganic perovskite solar cells(PSCs)are excellent top cell candidates in tandem applications.An essential challenge is the replacement of metal contacts with transparent co...Near-infrared(NIR)transparent inverted all-inorganic perovskite solar cells(PSCs)are excellent top cell candidates in tandem applications.An essential challenge is the replacement of metal contacts with transparent conductive oxide(TCO)electrodes,which requires the introduction of a buffer layer to prevent sputtering damage.In this study,we show that the conventional buffers(i.e.,small organic molecules and atomic layer deposited metal oxides)used for organic-inorganic hybrid perovskites are not applicable to all-inorganic perovskites,due to non-uniform coverage of the vulnerable layers underneath,deterioration upon ion bombardment and moisture induced perovskite phase transition,A thin film of metal oxide nanoparticles by the spin-coating method serves as a non-destructive buffer layer for inorganic PSCs.All-inorganic inverted near-infrared-transparent PSCs deliver a PCE of 17.46%and an average transmittance of 73.7%between 780 and 1200 nm.In combination with an 18.56%Cu(In,Ga)Se_(2) bottom cell,we further demonstrate the first all-inorganic perovskite/CIGS 4-T tandem solar cell with a PCE of 24.75%,which exhibits excellent illumination stability by maintaining 86.7%of its initial efficiency after 1400 h.The non-destructive buffer lays the foundation for efficient and stable NIR-transparent inverted inorganic perovskite solar cells and perovskite-based tandems.展开更多
Tunable bandgaps make halide perovskites promising candidates for developing tandem solar cells(TSCs),a strategy to break the radiative limit of 33.7%for single-junction solar cells.Combining perovskites with market-d...Tunable bandgaps make halide perovskites promising candidates for developing tandem solar cells(TSCs),a strategy to break the radiative limit of 33.7%for single-junction solar cells.Combining perovskites with market-dominant crystalline silicon(c-Si)is particularly attractive;simple estimates based on the bandgap matching indicate that the efficiency limit in such tandem device is as high as 46%.However,state-of-the-art perovskite/c-Si TSCs only achieve an efficiency of~32.5%,implying significant challenges and also rich opportunities.In this review,we start with the operating mechanism and efficiency limit of TSCs,followed by systematical discussions on wide-bandgap perovskite front cells,interface selective contacts,and electrical interconnection layer,as well as photon management for highly efficient perovskite/c-Si TSCs.We highlight the challenges in this field and provide our understanding of future research directions toward highly efficient and stable large-scale wide-bandgap perovskite front cells for the commercialization of perovskite/c-Si TSCs.展开更多
Compared with the power conversion efficicency,the operational stability of perovskite solar cells(PsCs)remains a major challenge hampering its commercialization.However,conducting a light soaking test under 1 sun ill...Compared with the power conversion efficicency,the operational stability of perovskite solar cells(PsCs)remains a major challenge hampering its commercialization.However,conducting a light soaking test under 1 sun illumination to get a long lifetime is time-consuming and experimentally inefficient.Here,we report an accelerated stability test protocol by aging PsCs under high-intensity light illumination to accelerate the evaluation of their operation stability.It is found that the efficiency degradation rate of a typical inverted PsC is almost linearly dependent on the light intensity within the range of 1 to 4 suns regardless of the encapsulations.The results prove that it can save the light-soaking time by at least 4 times to predict the operation lifetime on the basis of the equivalent light irradiation dose.展开更多
The high efficiency,solution processibility,and flexibility of perovskite solar cells make them promising candidates for the photovoltaic industry[1−8].The deposition method is one of the most critical factors that af...The high efficiency,solution processibility,and flexibility of perovskite solar cells make them promising candidates for the photovoltaic industry[1−8].The deposition method is one of the most critical factors that affect the performance of perovskite films.Various deposition methods have been developed to make perovskite films,including spin-coating,slotdie coating.展开更多
Perovskite solar cells(PSCs)with a positive-intrinsicnegative(p–i–n,commonly referred to as“inverted”)structure are becoming commercially attractive due to their superior power conversion efficiency(PCE)and better...Perovskite solar cells(PSCs)with a positive-intrinsicnegative(p–i–n,commonly referred to as“inverted”)structure are becoming commercially attractive due to their superior power conversion efficiency(PCE)and better operational stability as compared to the“normal”structure device.^([1–5])Nonetheless,further improvements in the device performance of inverted PSCs are hampered by interface losses,particularly where the buried interfaces are responsible for perovskite crystallization and chargecarrier extraction.^([6–9])展开更多
Metal halide perovskites are promising materials for solar cells because of high power conversion efficiency(PCE),tun-able bandgap,high defect tolerance,long carrier diffusion length,and low-cost fabrication[1-7].The ...Metal halide perovskites are promising materials for solar cells because of high power conversion efficiency(PCE),tun-able bandgap,high defect tolerance,long carrier diffusion length,and low-cost fabrication[1-7].The PCE for perovskite solar cells(PSCs)reaches 26.14%for single-junction cells,29.1%for perovskite/perovskite tandem cells and 33.9%for perovskite/silicon tandem cells,being comparable to that for silicon and other thin-film solar cells[8-10].Perovskite solar cells have been made by solution methods including spin-coat-ing,blade coating and printing[11,12].展开更多
The black-phase formamidine-lead iodide(α-FAPbI_(3)),boasting an optimal bandgap of 1.5 eV,stands out as a premier choice for narrow-bandgap perovskite solar cells(PSCs),achieving a certified power conversion efficie...The black-phase formamidine-lead iodide(α-FAPbI_(3)),boasting an optimal bandgap of 1.5 eV,stands out as a premier choice for narrow-bandgap perovskite solar cells(PSCs),achieving a certified power conversion efficiency(PCE)of 26.1%[1−5].This impressive performance hinges on the orderly and homogeneous crystallization ofα-phase pure FAPbI_(3),facilitated by coordinating solvents such as dimethyl sulfoxide(DMSO)to form intermediates like PbI_(2)-DMSO complex(D-complex).The D-complex plays a pivotal role in crystallization thermodynamics,enabling the direct formation of α-FAPbI_(3) without the photoinactiveδ-phase[6−9].However,DMSO,a commonly used coordinating solvent,is highly hygroscopic and prone to hydration upon moisture exposure.This tendency leads to incomplete perovskite crystallization and accelerates the transformation of α-FAPbI_(3) into itsδ-phase[2,10].Consequently,the best-performing α-FAPbI_(3)PSCs must be processed in an inert atmosphere with strictly controlled relative humidity(RH)and suffers from relatively poor reproducibility.Given the hard-to-control atmosphere at industrial scale,it is challenging yet imperative to eliminate the negative effects stemming from hygroscopic coordinating solvents[11−13].展开更多
Perovskite tandem solar cells(TSCs)are popular for their ability to surpass the Shockley-Queisser(S-Q)limit of singlejunction solar cells[1-9].Currently,there are mainly four types of perovskite TSCs,including perovsk...Perovskite tandem solar cells(TSCs)are popular for their ability to surpass the Shockley-Queisser(S-Q)limit of singlejunction solar cells[1-9].Currently,there are mainly four types of perovskite TSCs,including perovskite/silicon,perovskite/copper indium gallium selenide(CIGS).展开更多
基金the National Natural Science Foundation of China(62274138)Natural Science Foundation of Fujian Province of China(2023J06012)+2 种基金Science and Technology Plan Project in Fujian Province of China(2021H0011)Fundamental Research Funds for the Central Universities(20720230029)Compound semiconductor technology Collaborative Innovation Platform project of FuXiaQuan National Independent Innovation Demonstration Zone(3502ZCQXT2022005).
文摘In backlighting systems for liquid crystal displays,conventional red,green,and blue(RGB)light sources that lack polarization properties can result in a significant optical loss of up to 50%when passing through a polarizer.To address this inefficiency and optimize energy utilization,this study presents a high-performance device designed for RGB polarized emissions.The device employs an array of semipolar blueμLEDs with inherent polarization capabilities,coupled with mechanically stretched films of green-emitting CsPbBr3 nanorods and red-emitting CsPbI3-Cs4PbI6 hybrid nanocrystals.The CsPbBr3 nanorods in the polymer film offer intrinsic polarization emission,while the aligned-wire structures formed by the stable CsPbI3-Cs4PbI6 hybrid nanocrystals contribute to substantial anisotropic emissions,due to their high dielectric constant.The resulting device achieved RGB polarization degrees of 0.26,0.48,and 0.38,respectively,and exhibited a broad color gamut,reaching 137.2%of the NTSC standard and 102.5%of the Rec.2020 standard.When compared to a device utilizing c-plane LEDs for excitation,the current approach increased the intensity of light transmitted through the polarizer by 73.6%.This novel fabrication approach for polarized devices containing RGB components holds considerable promise for advancing next-generation display technologies.
基金financial support from the National Natural Science Foundation of China (52203070)the Open Fund of State Key Laboratory of New Textile Materials and Advanced Processing Technologies (FZ2022005)+2 种基金the Open Fund of Hubei Key Laboratory of Biomass Fiber and Ecological Dyeing and Finishing (STRZ202203)the financial support provided by the China Scholarship Council (CSC)Visiting Scholar Programfinancial support from Institute for Sustainability,Energy and Resources,The University of Adelaide,Future Making Fellowship,Australia。
文摘The incorporation of partial A-site substitution in perovskite oxides represents a promising strategy for precisely controlling the electronic configuration and enhancing its intrinsic catalytic activity.Conventional methods for A-site substitution typically involve prolonged high-temperature processes.While these processes promote the development of unique nanostructures with highly exposed active sites,they often result in the uncontrolled configuration of introduced elements.Herein,we present a novel approach for synthesizing two-dimensional(2D)porous GdFeO_(3) perovskite with A-site strontium(Sr)substitution utilizing microwave shock method.This technique enables precise control of the Sr content and simultaneous construction of 2D porous structures in one step,capitalizing on the advantages of rapid heating and cooling(temperature~1100 K,rate~70 K s^(-1)).The active sites of this oxygen-rich defect structure can be clearly revealed through the simulation of the electronic configuration and the comprehensive analysis of the crystal structure.For electrocatalytic oxygen evolution reaction application,the synthesized 2D porous Gd_(0.8)Sr_(0.2)FeO_(3) electrocatalyst exhibits an exceptional overpotential of 294 mV at a current density of 10 mA cm^(-2)and a small Tafel slope of 55.85 mV dec^(-1)in alkaline electrolytes.This study offers a fresh perspective on designing crystal configurations and the construction of nanostructures in perovskite.
基金the supports from the National Natural Science Foundation of China(Nos.62264012,62164009)Inner Mongolia Higher Education Research Project(No.NJZZ22343)+1 种基金Inner Mongolia University Research Foundation for Advanced Talents in 2021(No.10000-21311201/005)the Inner Mongolia Autonomous Region for Advanced Talents in 2020(No.12000-12102628)。
文摘Wide bandgap perovskite solar cells(PSCs)have attracted significant attention because they can be applied to the top cells of tandem solar cells.However,high open-circuit voltage(V_(OC))deficit(>0.4 V)result from poor crystallization and high non-radiative recombination losses become a serious limitation in the pursuit of high performance.Here,the relevance between different Pbl_(2)proportions and performance parameters are revealed through analysis of surface morphology,residual stress,and photostability.The increase of Pbl_(2)proportion promotes crystal growth and reduces the work function of the perovskite film surface and promotes the energy level alignment with the carrier transport layer,which decreased the V_(OC)deficit.However,residual PbI_(2)exacerbated the stress level of perovskite film,and the resulting lattice disorder deteriorated the photostability of the device.Ultimately,after the synergistic passivation of residual PbI_(2)and PEAI,the V_(OC)achieves 1.266 V and V_(OC)deficit is less than 0.4 V,the record value in wide bandgap PSCs.
文摘NiO_(x)as a hole transport material for inverted perovskite solar cells has received great attention owing to its high transparency,low fabrication temperature,and superior stability.However,the mismatched energy levels and possible redox reactions at the NiO_(x)/perovskite interface severely limit the performance of NiO_(x) based inverted perovskite solar cells.Herein,we introduce a p-type self-assembled monolayer between NiO_(x)and perovskite layers to modify the interface and block the undesirable redox reaction between perovskite and NiO_(x)The selfassembled monolayer molecules all contain phosphoric acid function groups,which can be anchored onto the NiOr surface and passivate the surface defect.Moreover,the introduction of self-assembled monolayers can regulate the energy level structure of NiO_(x),reduce the interfacial band energy offset,and hence promote the hole transport from perovskite to NiO_(x)layer.Consequently,the device performance is significantly enhanced in terms of both power conversion efficiency and stability.
基金supported by the National Natural Science Foundation of China(22279025,21773048)the Natural Science Foundation of Heilongjiang Province(LH2021A013)+1 种基金the Sichuan Science and Technology Program(2021YFSY0022)the Fundamental Research Funds for the Central Universities(2023FRFK06005,HIT.NSRIF202204)。
文摘Developing efficient and stable cathodes for low-temperature solid oxide fuel cells(LT-SOFCs) is of great importance for the practical commercialization.Herein,we propose a series of Sm-modified Bi_(0.7-x)Sm_xSr_(0.3)FeO_(3-δ) perovskites as highly-active catalysts for LT-SOFCs.Sm doping can significantly enhance the electrocata lytic activity and chemical stability of cathode.At 600℃,Bi_(0.675)Sm_(0.025)Sr_(0.3)FeO_(3-δ)(BSSF25) cathode has been found to be the optimum composition with a polarization resistance of 0.098 Ω cm^2,which is only around 22.8% of Bi_(0.7)Sr_(0.3)FeO_(3-δ)(BSF).A full cell utilizing BSSF25 displays an exceptional output density of 790 mW cm^(-2),which can operate continuously over100 h without obvious degradation.The remarkable electrochemical performance observed can be attributed to the improved O_(2) transport kinetics,superior surface oxygen adsorption capacity,as well as O_(2)p band centers in close proximity to the Fermi level.Moreover,larger average bonding energy(ABE) and the presence of highly acidic Bi,Sm,and Fe ions restrict the adsorption of CO_(2) on the cathode surface,resulting in excellent CO_(2) resistivity.This work provides valuable guidance for systematic design of efficient and durable catalysts for LT-SOFCs.
基金supported by the National Key Research and Development Program of China(2022YFB4200301)the National Natural Science Foundation of China(52202216)the Natural Science Foundation of Sichuan Province(24NSFSC1601).
文摘The use of low-dimensional(LD)perovskite materials is crucial for achieving high-performance perovskite solar cells(PSCs).However,LD perovskite films fabricated by conventional approaches give rise to full coverage of the underlying 3D perovskite films,which inevitably hinders the transport of charge carriers at the interface of PSCs.Here,we designed and fabricated LD perovskite structure that forms net-like morphology on top of the underlying three-dimensional(3D)perovskite bulk film.The net-like LD perovskite not only reduced the surface defects of 3D perovskite film,but also provided channels for the vertical transport of charge carriers,effectively enhancing the interfacial charge transfer at the LD/3D hetero-interface.The net-like morphological design comprising LD perovskite effectively resolves the contradiction between interfacial defect passivation and carrier extraction across the hetero-interfaces.Furthermore,the net-like LD perovskite morphology can enhance the stability of the underlying 3D perovskite film,which is attributed to the hydrophobic nature of LD perovskite.As a result,the net-like LD perovskite film morphology assists PSCs in achieving an excellent power conversion efficiency of up to 24.6%with over 1000 h long-term operational stability.
基金financial support from the National Natural Science Foundation of China(grant nos.52172198,51902117,and 91733301)。
文摘Solution processability significantly advances the development of highly-efficient perovskite solar cells.However,the precursor solution tends to undergo irreversible degradation reactions,impairing the device performance and reproducibility.Here,we utilize a reductive natural amino acid,Nacetylcysteine(NALC),to stabilize the precursor solution for printable carbon-based hole-conductorfree mesoscopic perovskite solar cells.We find that I_(2) can be generated in the aged solution containing methylammonium iodide(MI) in an inert atmosphere and speed up the MA-FA^(+)(formamidinium) reaction which produces large-size cations and hinders the formation of perovskite phase.NALC effectively stabilizes the precursor via its sulfhydryl group which reduces I_(2) back to I^(-)and provides H^(+).The NALC-stabilized precursor which is aged for 1440 h leads to devices with a power conversion efficiency equivalent to 98% of that for devices prepared with the fresh precursor.Furthermore,NALC improves the device power conversion efficiency from 16.16% to 18.41% along with enhanced stability under atmospheric conditions by modifying grain boundaries in perovskite films and reducing associated defects.
基金financially supported by the Natural Science Foundation of China(Grant Nos.52372226,52173263,62004167)the Natural Science Basic Research Plan in Shaanxi Province of China(Grant Nos.2022JM-315,2023-JC-QN-0643)+4 种基金the National Key R&D Program of China(Grant No.2022YFB3603703)the Qinchuangyuan High-level Talent Project of Shaanxi(Grant No.QCYRCXM-2022-219)the Ningbo Natural Science Foundation(Grant No.2022J061)the Key Research and Development Program of Shaanxi(Grant No.2023GXLH-091)the Shccig-Qinling Program and the Fundamental Research Funds for the Central Universities。
文摘Two-dimensional Ruddlesden-Popper(2DRP)perovskite exhibits excellent stability in perovskite solar cells(PSCs)due to introducing hydrophobic long-chain organic spacers.However,the poor charge transporting property of bulky organic cation spacers limits the performance of 2DRP PSCs.Inspired by the Asite cation alloying strategy in 3D perovskites,2DRP perovskites with a binary spacer can promote charge transporting compared to the unary spacer counterparts.Herein,the superior MA-based 2DRP perovskite films with a binary spacer,including 3-guanidinopropanoic acid(GPA)and 4-fluorophenethylamine(FPEA)are realized.These films(GPA_(0.85)FPEA_(0.15))_(2)MA_(4)Pb_5I_(16)show good morphology,large grain size,decreased trap state density,and preferential orientation of the as-prepared film.Accordingly,the present 2DRP-based PSC with the binary spacer achieves a remarkable efficiency of 18.37%with a V_(OC)of1.15 V,a J_(SC)of 20.13 mA cm^(-2),and an FF of 79.23%.To our knowledge,the PCE value should be the highest for binary spacer MA-based 2DRP(n≤5)PSCs to date.Importantly,owing to the hydrophobic fluorine group of FPEA and the enhanced interlayer interaction by FPEA,the unencapsulated 2DRP PSCs based on binary spacers exhibit much excellent humidity stability and thermal stability than the unary spacer counterparts.
基金the financial support from Shanxi Province Science and Technology Department(20201101012,202101060301016)the support from the APRC Grant of the City University of Hong Kong(9380086)+5 种基金the TCFS Grant(GHP/018/20SZ)MRP Grant(MRP/040/21X)from the Innovation and Technology Commission of Hong Kongthe Green Tech Fund(202020164)from the Environment and Ecology Bureau of Hong Kongthe GRF grants(11307621,11316422)from the Research Grants Council of Hong KongGuangdong Major Project of Basic and Applied Basic Research(2019B030302007)Guangdong-Hong Kong-Macao Joint Laboratory of Optoelectronic and Magnetic Functional Materials(2019B121205002).
文摘A considerable efficiency gap exists between large-area perovskite solar modules and small-area perovskite solar cells.The control of forming uniform and large-area film and perovskite crystallization is still the main obstacle restricting the efficiency of PSMs.In this work,we adopted a solid-liquid two-step film formation technique,which involved the evaporation of a lead iodide film and blade coating of an organic ammonium halide solution to prepare perovskite films.This method possesses the advantages of integrating vapor deposition and solution methods,which could apply to substrates with different roughness and avoid using toxic solvents to achieve a more uniform,large-area perovskite film.Furthermore,modification of the NiO_(x)/perovskite buried interface and introduction of Urea additives were utilized to reduce interface recombination and regulate perovskite crystallization.As a result,a large-area perovskite film possessing larger grains,fewer pinholes,and reduced defects could be achieved.The inverted PSM with an active area of 61.56 cm^(2)(10×10 cm^(2)substrate)achieved a champion power conversion efficiency of 20.56%and significantly improved stability.This method suggests an innovative approach to resolving the uniformity issue associated with large-area film fabrication.
基金supported by the National Research Foundation of Korea funded by the Ministry of Science and ICT (MSIT),Korea (NRF-2021R1C1C1009200 and 2023R1A2C3007358)supported by the Defense Challengeable Future Technology Program of the Agency for Defense Development,Republic of Koreasupported by Technology Innovation Program of the Korea Evaluation Institute of Industrial Technology (KEIT) (20016588)funded by Ministry of Trade,Industry and Energy (MOTIE).
文摘The successful utilization of an eco-friendly and biocompatible parylene-C substrate for high-performance solution-processed double-walled carbon nanotube(CNT)electrode-based perovskite solar cells(PSCs)was demonstrated.Through the use of a novel inversion transfer technique,vertical separation of the binders from the CNTs was induced,rendering a stronger p-doping effect and thereby a higher conductivity of the CNTs.The resulting foldable devices exhibited a power conversion efficiency of 18.11%,which is the highest reported among CNT transparent electrode-based PSCs to date,and withstood more than 10,000 folding cycles at a radius of 0.5 mm,demonstrating unprecedented mechanical stability.Furthermore,solar modules were fabricated using entirely laser scribing processes to assess the potential of the solution-processable nanocarbon electrode.Notably,this is the only one to be processed entirely by the laser scribing process and to be biocompatible as well as eco-friendly among the previously reported nonindium tin oxide-based perovskite solar modules.
基金financially supported by the National Natural Science Foundation of China(51902110,U21A2078,and 22179042)Natural Science Foundation of Fujian Province(2020J01064 and 2020J06021)Scientific Research Funds of Huaqiao University,and the Promotion Program for Young and Middle-aged Teacher in Science and Technology Research of Huaqiao University(ZQN-806,ZQNPY607)
文摘Tin-based perovskite solar cells(TPSCs)have received great attention due to their eco-friendly properties and high theoretical efficiencies.However,the fast crystallization feature of tin-based perovskites leads to poor film quality and limits the corresponding device performance.Herein,a chlorofullerene,C_(60)Cl_(6),with six chlorine attached to the C_(60)cage,is applied to modulate the crystallization process and passivate grain boundary defects of the perovskite film.The chemical interactions between C_(60)Cl_(6)and perovskite components retard the transforming process of precursors to perovskite crystals and obtain a high-quality tin-based perovskite film.It is also revealed that the C_(60)Cl_(6)located at the surfaces and grain boundaries can not only passivate the defects but also offer a role in suturing grain boundaries to suppress the detrimental effects of water and oxygen on perovskite films,especially the oxidation of Sn^(2+)to Sn^(4+).As a result,the C_(60)Cl_(6)-based device yields a remarkably improved device efficiency from 10.03%to 13.30%with enhanced stability.This work provides a new strategy to regulate the film quality and stability of TPSCs using functional fullerene materials.
基金supported by the National Key Research and Development Program of China(Grant Nos.2021YFA1400200 and2021YFA0718701)the National Natural Science Foundation of China(Grant Nos.U2032127,11904322,12104411,12174347)+4 种基金the Natural Science Foundation of Henan province of China(Grant No.202300410356)the China Postdoctoral Science Foundation(Grant Nos.2019M652560 and 2020M682326)the CAS Interdisciplinary Innovation Team(Grant No.JCTD-2019-01)the Postdoctoral Research Grant in Henan Province(Grant No.1902013)the Science Foundation for Highlevel Talents of Wuyi University(Grant No.2021AL019)。
文摘The Cs_(2)NaInCl_(6) double perovskite is one of the most promising lead-free perovskites due to its exceptional stability and straightforward synthesis.However,it faces challenges related to inefficient photoluminescence.Doping and high pressure are employed to tailor the optical properties of Cs_(2)NaInCl_(6).Herein,Sb^(3+)doped Cs_(2)NaInCl_(6)(Sb^(3+):Cs_(2)NaInCl_(6)) was synthesized and it exhibits blue emission with a photoluminescence quantum yield of up to 37.3%.Further,by employing pressure tuning,a blue stable emission under a very wide range from 2.7 GPa to 9.8 GPa is realized in Sb^(3+):Cs_(2)NaInCl_(6).Subsequently,the emission intensity of Sb^(3+):Cs_(2)NaInCl_(6) experiences a significant increase(3.3 times)at 19.0 GPa.It is revealed that the pressure-induced distinct emissions can be attributed to the carrier self-trapping and detrapping between Cs_(2)NaInCl_(6) and Sb^(3+).Notably,the lattice compression in the cubic phase inevitably modifies the band gap of Sb^(3+):Cs_(2)NaInCl_(6).Our findings provide valuable insights into effects of the high pressure in further boosting unique emission characteristics but also offer promising opportunities for development of doped double perovskites with enhanced optical functionalities.
基金financially supported by the National Natural Science Foundation of China (22279083,22109166,52202183)Guangdong Basic and Applied Basic Research Foundation (Grant No.2019A1515011136,2022B1515120006,2023B1515120041,2414050001473)+3 种基金Guangdong Province Higher Vocational Colleges and Schools Pearl River Scholar Funded SchemeGuangdong Provincial Key Laboratory Program (2021B1212040001)from the Department of Science and Technology of Guangdong ProvinceBeijing Institute of TechnologySongshan Lake Materials Laboratory。
文摘Near-infrared(NIR)transparent inverted all-inorganic perovskite solar cells(PSCs)are excellent top cell candidates in tandem applications.An essential challenge is the replacement of metal contacts with transparent conductive oxide(TCO)electrodes,which requires the introduction of a buffer layer to prevent sputtering damage.In this study,we show that the conventional buffers(i.e.,small organic molecules and atomic layer deposited metal oxides)used for organic-inorganic hybrid perovskites are not applicable to all-inorganic perovskites,due to non-uniform coverage of the vulnerable layers underneath,deterioration upon ion bombardment and moisture induced perovskite phase transition,A thin film of metal oxide nanoparticles by the spin-coating method serves as a non-destructive buffer layer for inorganic PSCs.All-inorganic inverted near-infrared-transparent PSCs deliver a PCE of 17.46%and an average transmittance of 73.7%between 780 and 1200 nm.In combination with an 18.56%Cu(In,Ga)Se_(2) bottom cell,we further demonstrate the first all-inorganic perovskite/CIGS 4-T tandem solar cell with a PCE of 24.75%,which exhibits excellent illumination stability by maintaining 86.7%of its initial efficiency after 1400 h.The non-destructive buffer lays the foundation for efficient and stable NIR-transparent inverted inorganic perovskite solar cells and perovskite-based tandems.
基金the talent project of ZJU-Hangzhou Global Scientific and Technological Innovation Center(No.02170000-K02013017)project of National Natural Science Foundation of China(No.61721005)
文摘Tunable bandgaps make halide perovskites promising candidates for developing tandem solar cells(TSCs),a strategy to break the radiative limit of 33.7%for single-junction solar cells.Combining perovskites with market-dominant crystalline silicon(c-Si)is particularly attractive;simple estimates based on the bandgap matching indicate that the efficiency limit in such tandem device is as high as 46%.However,state-of-the-art perovskite/c-Si TSCs only achieve an efficiency of~32.5%,implying significant challenges and also rich opportunities.In this review,we start with the operating mechanism and efficiency limit of TSCs,followed by systematical discussions on wide-bandgap perovskite front cells,interface selective contacts,and electrical interconnection layer,as well as photon management for highly efficient perovskite/c-Si TSCs.We highlight the challenges in this field and provide our understanding of future research directions toward highly efficient and stable large-scale wide-bandgap perovskite front cells for the commercialization of perovskite/c-Si TSCs.
基金financially supported by the Ministry of Science and Technology of China (2021YFB3800104)the National Natural Science Foundation of China (52002140, U20A20252)+3 种基金the Young Elite Scientists Sponsorship Program by CASTthe Selfdetermined and Innovative Research Funds of HUST(2020kfyXJJS008)the Natural Science Foundation of Hubei Province (2022CFA093)the Innovation Project of Optics Valley Laboratory (Grant No. OVL2021BG008)
文摘Compared with the power conversion efficicency,the operational stability of perovskite solar cells(PsCs)remains a major challenge hampering its commercialization.However,conducting a light soaking test under 1 sun illumination to get a long lifetime is time-consuming and experimentally inefficient.Here,we report an accelerated stability test protocol by aging PsCs under high-intensity light illumination to accelerate the evaluation of their operation stability.It is found that the efficiency degradation rate of a typical inverted PsC is almost linearly dependent on the light intensity within the range of 1 to 4 suns regardless of the encapsulations.The results prove that it can save the light-soaking time by at least 4 times to predict the operation lifetime on the basis of the equivalent light irradiation dose.
基金We thank the National Natural Science Foundation of China(52203217 and 21961160720)the National Key Research and Development Program of China(2022YFB3803300)the open research fund of Songshan Lake Materials Laboratory(2021SLABFK02)for financial support.
文摘The high efficiency,solution processibility,and flexibility of perovskite solar cells make them promising candidates for the photovoltaic industry[1−8].The deposition method is one of the most critical factors that affect the performance of perovskite films.Various deposition methods have been developed to make perovskite films,including spin-coating,slotdie coating.
文摘Perovskite solar cells(PSCs)with a positive-intrinsicnegative(p–i–n,commonly referred to as“inverted”)structure are becoming commercially attractive due to their superior power conversion efficiency(PCE)and better operational stability as compared to the“normal”structure device.^([1–5])Nonetheless,further improvements in the device performance of inverted PSCs are hampered by interface losses,particularly where the buried interfaces are responsible for perovskite crystallization and chargecarrier extraction.^([6–9])
基金We thank the Key Research and Development Project of Anhui Province(2023t07020005)Natural Science Foundation of Anhui Province(2308085QE137)+2 种基金Anhui Innovation&Entrepreneurship Support Plan for Returned Overseas Students(2022LCX018)L.Ding thanks the Nation al Key Research and Development Program of China(2022YFB3803300,2023YFE0116800)Beijing Natural Science Foundation(IS23037).
文摘Metal halide perovskites are promising materials for solar cells because of high power conversion efficiency(PCE),tun-able bandgap,high defect tolerance,long carrier diffusion length,and low-cost fabrication[1-7].The PCE for perovskite solar cells(PSCs)reaches 26.14%for single-junction cells,29.1%for perovskite/perovskite tandem cells and 33.9%for perovskite/silicon tandem cells,being comparable to that for silicon and other thin-film solar cells[8-10].Perovskite solar cells have been made by solution methods including spin-coat-ing,blade coating and printing[11,12].
基金support from the National Natural Science Foundation of China(Grant Nos.62205154 and 62288102)the Natural Science Research Start-up Foundation of Recruiting Talents of Nanjing University of Posts and Telecommunications(Grant No.NY221112).
文摘The black-phase formamidine-lead iodide(α-FAPbI_(3)),boasting an optimal bandgap of 1.5 eV,stands out as a premier choice for narrow-bandgap perovskite solar cells(PSCs),achieving a certified power conversion efficiency(PCE)of 26.1%[1−5].This impressive performance hinges on the orderly and homogeneous crystallization ofα-phase pure FAPbI_(3),facilitated by coordinating solvents such as dimethyl sulfoxide(DMSO)to form intermediates like PbI_(2)-DMSO complex(D-complex).The D-complex plays a pivotal role in crystallization thermodynamics,enabling the direct formation of α-FAPbI_(3) without the photoinactiveδ-phase[6−9].However,DMSO,a commonly used coordinating solvent,is highly hygroscopic and prone to hydration upon moisture exposure.This tendency leads to incomplete perovskite crystallization and accelerates the transformation of α-FAPbI_(3) into itsδ-phase[2,10].Consequently,the best-performing α-FAPbI_(3)PSCs must be processed in an inert atmosphere with strictly controlled relative humidity(RH)and suffers from relatively poor reproducibility.Given the hard-to-control atmosphere at industrial scale,it is challenging yet imperative to eliminate the negative effects stemming from hygroscopic coordinating solvents[11−13].
基金support from the National University Research Fund(GK202309020)the Young Scientist Initiative Project of School of Materials Science and Engineering at Shaanxi Normal University(2023YSIP-MSESNNU002)Open Fund of National Laboratory of Solid State Microstructures,Nanjing University。
文摘Perovskite tandem solar cells(TSCs)are popular for their ability to surpass the Shockley-Queisser(S-Q)limit of singlejunction solar cells[1-9].Currently,there are mainly four types of perovskite TSCs,including perovskite/silicon,perovskite/copper indium gallium selenide(CIGS).