Ni-Fe-based oxides are among the most promising catalysts developed to date for the bottleneck oxygen evolution reaction(OER)in water electrolysis.However,understanding and mastering the synergy of Ni and Fe remain ch...Ni-Fe-based oxides are among the most promising catalysts developed to date for the bottleneck oxygen evolution reaction(OER)in water electrolysis.However,understanding and mastering the synergy of Ni and Fe remain challenging.Herein,we report that the synergy between Ni and Fe can be tailored by crystal dimensionality of Ni,Fe-contained Ruddlesden-Popper(RP)-type perovskites(La_(0.125)Sr_(0.875))n+1(Ni_(0.25)Fe_(0.75))nO3n+1(n=1,2,3),where the material with n=3 shows the best OER performance in alkaline media.Soft X-ray absorption spectroscopy spectra before and after OER reveal that the material with n=3 shows enhanced Ni/Fe-O covalency to boost the electron transfer as compared to those with n=1 and n=2.Further experimental investigations demonstrate that the Fe ion is the active site and the Ni ion is the stable site in this system,where such unique synergy reaches the optimum at n=3.Besides,as n increases,the proportion of unstable rock-salt layers accordingly decreases and the leaching of ions(especially Sr^(2+))into the electrolyte is suppressed,which induces a decrease in the leaching of active Fe ions,ultimately leading to enhanced stability.This work provides a new avenue for rational catalyst design through the dimensional strategy.展开更多
Wide-bandgap(>1.7 eV)perovskites suffer from severe light-induced phase segregation due to high bromine content,causing irreversible damage to devices stability.However,the strategies of suppressing photoinduced ph...Wide-bandgap(>1.7 eV)perovskites suffer from severe light-induced phase segregation due to high bromine content,causing irreversible damage to devices stability.However,the strategies of suppressing photoinduced phase segregation and related mechanisms have not been fully disclosed.Here,we report a new passivation agent 4-aminotetrahydrothiopyran hydrochloride(4-ATpHCl)with multifunctional groups for the interface treatment of a 1.77-eV wide-bandgap perovskite film.4-ATpH^(+)impeded halogen ion migration by anchoring on the perovskite surface,leading to the inhibition of phase segregation and thus the passivation of defects,which is ascribed to the interaction of 4-ATpH^(+)with perovskite and the formation of low-dimensional perovskites.Finally,the champion device achieved an efficiency of 19.32%with an open-circuit voltage(V_(OC))of 1.314 V and a fill factor of 83.32%.Moreover,4-ATpHCl modified device exhibited significant improved stability as compared with control one.The target device maintained 80%of its initial efficiency after 519 h of maximum power output(MPP)tracking under 1 sun illumination,however,the control device showed a rapid decrease in efficiency after 267 h.Finally,an efficiency of 27.38%of the champion 4-terminal all-perovskite tandem solar cell was achieved by mechanically stacking this wide-bandgap top subcell with a 1.25-eV low-bandgap perovskite bottom subcell.展开更多
Energy supply dominated by fossil energy has been and remains the main cause of carbon dioxide emissions,the major greenhouse gas leading to the current grave climate change challenges.Many technical pathways have bee...Energy supply dominated by fossil energy has been and remains the main cause of carbon dioxide emissions,the major greenhouse gas leading to the current grave climate change challenges.Many technical pathways have been proposed to address the challenges.Carbon capture and utilization(CCU) represents one of the approaches and thermochemical CO_(2) splitting driven by thermal energy is a subset of the CCU,which converts the captured CO_(2) into CO and makes it possible to achieve closed-loop carbon recirculation.Redox-active catalysts are among the most critical components of the thermochemical splitting cycles and perovskites are regarded as the most promising catalysts.Here we review the latest advancements in thermochemical cycles based on perovskites,covering thermodynamic principles,material modifications,reaction kinetics,oxygen pressure control,circular strategies,and demonstrations to provide a comprehensive overview of the topical area.Thermochemical cycles based on such materials require the consideration of trade-off between cost and efficiency,which is related to actual material used,operation mode,oxygen removal,and heat recovery.Lots of efforts have been made towards improving reaction rates,conversion efficiency and cycling stability,materials related research has been lacking-a key aspect affecting the performance across all above aspects.Double perovskites and composite perovskites arise recently as a potentially promising addition to material candidates.For such materials,more effective oxygen removal would be needed to enhance the overall efficiency,for which thermochemical or electrochemical oxygen pumps could contribute to efficient oxygen removal as well as serve as means for inert gas regeneration.The integration of thermochemical CO_(2) splitting process with downstream fuel production and other processes could reduce costs and increase efficiency of the technology.This represents one of the directions for the future research.展开更多
Wide-bandgap(WBG)perovskite solar cells(PSCs)play a fundamental role in perovskite-based tandem solar cells.However,the efficiency of WBG PSCs is limited by significant open-circuit voltage losses,which are primarily ...Wide-bandgap(WBG)perovskite solar cells(PSCs)play a fundamental role in perovskite-based tandem solar cells.However,the efficiency of WBG PSCs is limited by significant open-circuit voltage losses,which are primarily caused by surface defects.In this study,we present a novel method for modifying surfaces using the multifunctional S-ethylisothiourea hydrobromide(SEBr),which can passivate both Pb^(-1)and FA^(-1)terminated surfaces,Moreover,the SEBr upshifted the Fermi level at the perovskite interface,thereby promoting carrier collection.This proposed method was effective for both 1.67 and 1.77 eV WBG PSCs,achieving power conversion efficiencies(PCEs)of 22.47%and 19.90%,respectively,with V_(OC)values of 1.28 and 1.33 V,along with improved film and device stability.With this advancement,we were able to fabricate monolithic all-perovskite tandem solar cells with a champion PCE of 27.10%,This research offers valuable insights for passivating the surface trap states of WBG perovskite through rational multifunctional molecular engineering.展开更多
The next-generation hot-carrier solar cells,which can overcome the Shockley-Queisser limit by harvesting excessenergy from hot carriers,are receiving increasing attention.Lead halide perovskite(LHP)materials are consi...The next-generation hot-carrier solar cells,which can overcome the Shockley-Queisser limit by harvesting excessenergy from hot carriers,are receiving increasing attention.Lead halide perovskite(LHP)materials are considered aspromising candidates due to their exceptional photovoltaic properties,good stability and low cost.The cooling rate of hotcarriers is a key parameter influencing the performance of hot-carrier solar cells.In this work,we successfully detected hotcarrier dynamics in operando LHP devices using the two-pulse photovoltage correlation technique.To enhance the signalto-noise ratio,we applied the delay-time modulation method instead of the traditional power modulation.This advancementallowed us to detect the intraband hot carrier cooling time for the organic LHP CH_(3)NH_(3)PbBr_(3),which is as short as 0.21 ps.In comparison,the inorganic Cs-based LHP CsPbBr_(3)exhibited a longer cooling time of around 0.59 ps due to differentphonon contributions.These results provide us new insights into the optimal design of hot-carrier solar cells and highlightthe potential of LHP materials in advancing solar cell technology.展开更多
CsPbI_(2)Br perovskite solar cell has been extensively studied due to its exceptional thermal stability and relatively stable perovskite phase structure.However,the presence of bromine leads to a rapid crystallization...CsPbI_(2)Br perovskite solar cell has been extensively studied due to its exceptional thermal stability and relatively stable perovskite phase structure.However,the presence of bromine leads to a rapid crystallization rate of CsPbI_(2)Br films,resulting in small grain size and high defect density.Additionally,CsPbI_(2)Br demonstrates poor light absorption due to its wide bandgap.Therefore,it is crucial to control the crystallization rate and increase the film thickness to reduce defect density,enhance light absorption,and improve photovoltaic performance.In this study,we utilized a PbAc_(2)-incorporated twice spincoating(PTS) process to address these issues.Initially,PbAc_(2) was added to the CsPbI_(2)Br precursor solution to form a CsPbI_(2)Br film,which was then coated with the CsPbI_(2)Br precursor solution to produce the PTS film,Ac^(-)can delay the perovskite crystallization,leading to the formation of thicker and denser CsPbI_(2)Br films.Moreover,lone-pair electrons of the oxygen atom provided by Ac^(-)formed coordination bonds with under-coordinated Pb~(2+) ions to fill halogen ion vacancies,thereby reducing the defect density.Ultimately,the PTS CsPbI_(2)Br device achieved a peak power conversion efficiency(PCE) of 16.19% and maintained 96.7% of its initial PCE over 1500 h at room temperature under 25% relative humidity without any encapsulation.展开更多
The outcomes of computational study of electronic, magnetic and optical spectra for A2BX6 (A = Rb;B = Tc, Pb, Pt, Sn, W, Ir, Ta, Sb, Te, Se, Mo, Mn, Ti, Zr and X = Cl, Br) materials have been proceeded utilizing Vande...The outcomes of computational study of electronic, magnetic and optical spectra for A2BX6 (A = Rb;B = Tc, Pb, Pt, Sn, W, Ir, Ta, Sb, Te, Se, Mo, Mn, Ti, Zr and X = Cl, Br) materials have been proceeded utilizing Vanderbilt Ultra Soft Pseudo Potential (US-PP) process. The Rb2PbBr6 and Rb2PbCl6 are found to be a (Г-Г) semiconductors with energy gaps of 0.275 and 1.142 eV, respectively making them promising photovoltaic materials. The metallic behavior of the materials for Rb2BX6 (B = Tc, W, Ir, Ta, Mn, Sb, Mo) has been confirmed showing the attendance of conducting lineaments. The dielectric function is found to be large close to the ultraviolet districts (3.10 - 4.13 eV). The extinction coefficient of the Rb2BX6 has the ability to be used for implements. The band structures and density of states ensure the magnetic semiconductors’ nature of the Rb2Mn (Cl, Br)6 perovskites. The total calculated magnetic moment of Rb2MnCl6 and Rb2MnB6 is 3.00μβ. Advanced spintronic technology requires room-temperature ferromagnetism. The present work confirms that, bromine and chlorine-founded double perovskites are extremely attractive for photovoltaic and optoelectronic devices.展开更多
Organic-inorganic halides perovskites(OHPs)have drawn the attention of many researchers owing to their astonishing and unique optoelectronic properties.They have been extensively used for photovoltaic applications,ach...Organic-inorganic halides perovskites(OHPs)have drawn the attention of many researchers owing to their astonishing and unique optoelectronic properties.They have been extensively used for photovoltaic applications,achieving higher than 26%power conversion efficiency to date.These materials have potential to be deployed for many other applications beyond photovoltaics like photodetectors,sensors,light-emitting diodes(LEDs),and resistors.To address the looming challenge of Moore’s law and the Von Neumann bottleneck,many new technologies regarding the computation of architectures and storage of information are being extensively researched.Since the discovery of the memristor as a fourth component of the circuit,many materials are explored for memristive applications.Lately,researchers have advanced the exploration of OHPs for memristive applications.These materials possess promising memristive properties and various kinds of halide perovskites have been used for different applications that are not only limited to data storage but expand towards artificial synapses,and neuromorphic computing.Herein we summarize the recent advancements of OHPs for memristive applications,their unique electronic properties,fabrication of materials,and current progress in this field with some future perspectives and outlooks.展开更多
The development of tin-based devices with low toxicity is critical for the commercial viability of perovskite solar cells.However because tin halide is a stronger Lewis acid,its crystallization rate is extremely fast,...The development of tin-based devices with low toxicity is critical for the commercial viability of perovskite solar cells.However because tin halide is a stronger Lewis acid,its crystallization rate is extremely fast,resulting in the formation of numerous defects that affect the device performance of tin-based perovskite solar cells.Herein,propylamine hydrobromide(PABr)was added to the perovskite precursor solution as an additive to passivate defects and fabricate more uniform and dense perovskite films.Because propylamine cations are too large to enter the perovskite lattices,they only exist at the grain boundary to passivate surface defects and promote crystal growth in a preferred orientation.The PABr additive raises the average short-circuit current density from 19.45 to 25.47 mA·cm^(-2)by reducing carrier recombination induced by defects.Furthermore,the device’s long-term illumination stability is improved after optimization,and the hysteresis effect is negligible.The addition of PABr results in a power conversion efficiency of 9.35%.展开更多
Energetic molecular perovskites have attracted widespread attention in the fields of energy materials due to their high detonation performance.In this work,we reported the effect of MgCo_(2)O_(4) nanosheets on the the...Energetic molecular perovskites have attracted widespread attention in the fields of energy materials due to their high detonation performance.In this work,we reported the effect of MgCo_(2)O_(4) nanosheets on the thermal decomposition of ammonium perchlorate(NH_(4)ClO_(4),AP)-based energetic molecular perovskites(AP-based energetic molecular perovskites).The morphology and structure of the MgCo_(2)O_(4) nanosheets were characterized.And their catalytic effect on the thermal decomposition of AP-based energetic molecular perovskites(H_2pz)[NH_(4)(ClO_(4))_(3)](PAP-4),(H_2dabco)[NH_(4)(ClO_(4))_(3)](DAP-4),(H_2mpz)[NH_(4)(ClO_(4))_(3)](PAP-M_(4)),and (H_2hpz)[NH_(4)(ClO_(4))_(3)](PAP-H_(4)) was analyzed.The results showed that MgCo_(2)O_(4) nanosheets had excellent intrinsically catalytic performance towards enhancing the thermal decomposition of AP-based energetic molecular perovskites.After adding MgCo_(2)O_(4) nanosheets,the thermal decomposition peak temperatures of PAP-4,DAP-4,PAP-M_(4),and PAP-H_(4) had been reduced by35.7℃,48.4℃,37.9℃,and 43.6℃,respectively.And the activation energy(Ea)of the thermal decomposition of AP-based energetic molecular perovskites had been reduced,the Eaof PAP-H_(4) decreased by 46.4 kJ/mol at most among them.The catalytic mechanism of MgCo_(2)O_(4) nanosheets for AP-based energetic molecular perovskites is analyzed.This work provides a reference for the future application of AP-based energetic molecular perovskites.展开更多
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
Hybrid lead halide perovskites have received great attention in the field of light-emitting diodes(LEDs)owing to their excellent optoelectronic properties,low cost,and high color purity.To data,the external quantum ef...Hybrid lead halide perovskites have received great attention in the field of light-emitting diodes(LEDs)owing to their excellent optoelectronic properties,low cost,and high color purity.To data,the external quantum efficiency(EQE)of lead halide perovskites LEDs has been reported to exceed 20%[1].Even so,the toxicity of conventional lead has cast a gloomy shadow over their further application.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
The formation of Frohlich polarons in metal halide perovskites,arising from the charge carrier-longitudinal optical(LO)phonon coupling,has been proposed to explain their exceptional properties,but the effective identi...The formation of Frohlich polarons in metal halide perovskites,arising from the charge carrier-longitudinal optical(LO)phonon coupling,has been proposed to explain their exceptional properties,but the effective identification of polarons in these materials is still a challenging task.Herein,we theoretically present the infrared optical absorption of Frohlich polarons based on the Huang-Rhys model.We find that multiphonon overtones appear as the energy of the incident photons matches the multiple LO phonons,wherein the average phonon number of a polaron can be directly evaluated by the order of the strongest overtone.These multiphonon structures sensitively depend on the scale of electronic distribution in the ground state and the dimensionality of the perovskite materials,revealing the effective modulation of competing processes between polaron formation and carrier cooling.Moreover,the order of the strongest overtone shifts to higher ones with temperature,providing a potential proof that the carrier mobility is affected by LO phonon scattering.The present model not only suggests a direct way to verify Frohlich polarons but also enriches our understanding of the properties of polarons in metal halide perovskites.展开更多
Perovskite solar cells(PSCs) as a rising star in the photovoltaic field have received rapidly increasing attention recently due to the boosting power conversion efficiencies(PCEs) from 3.8% to 25.7% in the last13 year...Perovskite solar cells(PSCs) as a rising star in the photovoltaic field have received rapidly increasing attention recently due to the boosting power conversion efficiencies(PCEs) from 3.8% to 25.7% in the last13 years. Nevertheless, the conventional PSCs with three-dimensional(3D) halide perovskites as light absorbers suffer from inferior PCEs and poor durability under sunlight, high-temperature and humid conditions due to the high defect amount and structural instability of 3D perovskites, respectively. To tackle these crucial issues, lower-dimensional halide perovskites including zero-dimensional(0D), onedimensional(1D), and two-dimensional(2D) perovskites have been employed as efficient passivators to boost the PCEs and durability of 3D-PSCs due to the high structural stability and superior resistance against moisture, heat and sunlight. Therefore, in order to achieve better understanding about the advantages and superiorities of combining low-dimensional perovskites with their 3D counterparts in improving the PCEs and durability of 3D-PSCs, the recent advances in the development and fabrication of mixeddimensional PSCs with 1D/0D perovskites as passivators are summarized and discussed in the review.The superiority of 1D/0D perovskites as passivators over 2D counterparts, the passivation mechanism and the methods of 1D/0D perovskites are also presented and discussed. Furthermore, the rules to choose1D/0D perovskites or relevant spacer cations are also emphasized. On this basis, several specific strategies to design and fabricate mixed-dimensional PSCs with 1D/0D perovskites are presented and discussed.Finally, the crucial challenges and future research directions of mixed-dimensional PSCs with 1D/0D perovskites as passivators are also proposed and discussed. This review will provide some useful insights for the future development of high-efficiency and durable mixed-dimensional PSCs.展开更多
Wide-bandgap(WBG)perovskites have been attracting much attention because of their immense potential as a front light-absorber for tandem solar cells.However,WBG perovskite solar cells(PSCs)generally exhibit undesired ...Wide-bandgap(WBG)perovskites have been attracting much attention because of their immense potential as a front light-absorber for tandem solar cells.However,WBG perovskite solar cells(PSCs)generally exhibit undesired large open-circuit voltage(VOC)loss due to light-induced phase segregation and severe non-radiative recombination loss.Herein,antimony potassium tartrate(APTA)is added to perovskite precursor as a multifunctional additive that not only coordinates with unbonded lead but also inhibits the migration of halogen in perovskite,which results in suppressed non-radiative recombination,inhibited phase segregation and better band energy alignment.Therefore,a APTA auxiliary WBG PSC with a champion photoelectric conversion efficiency of 20.35%and less hysteresis is presented.They maintain 80%of their initial efficiencies under 100 mW cm^(-2)white light illumination in nitrogen after 1,000 h.Furthermore,by combining a semi-transparent WBG perovskite front cell with a narrow-bandgap tin–lead PSC,a perovskite/perovskite four-terminal tandem solar cell with an efficiency over 26%is achieved.Our work provides a feasible approach for the fabrication of efficient tandem solar cells.展开更多
Lead(Pb)-free halide perovskites have recently attracted increasing attention as potential catalysts for CO_(2) photoreduction to CO due to their potential to capture solar energy and drive catalytic reaction.However,...Lead(Pb)-free halide perovskites have recently attracted increasing attention as potential catalysts for CO_(2) photoreduction to CO due to their potential to capture solar energy and drive catalytic reaction.However,issues of the poor charge transfer still remain one of the main obstacles limiting their performance due to the overwhelming radiative and nonradiative charge-carrier recombination losses.Herein,Pb-free Sb-alloyed all-inorganic quadruple perovskite Cs_(4)Mn(Bi_(1-x)Sb_(x))_(2)Cl_(12)(0≤x≤1)is synthesized as efficient photocatalyst.By Sb alloying,the undesired relaxation of photogenerated electrons from conduction band to emission centers of[MnCl6]^(4-)is greatly suppressed,resulting in a weakened PL emission and enhanced charge transfer for photocatalyst.The ensuing Cs_(4)Mn(Bi_(1-x)Sb_(x))_(2)Cl_(12) photocatalyst accomplishes efficient conversion of CO_(2)into CO,accompanied by a surprising production of H_(2)O_(2),a high valueadded product associated with water oxidation.By optimizing Sb^(3+) concentration,a high CO evolution rate of 35.1μmol g^(-1)h^(-1)is achieved,superior to most other Pb and Pb-free halide perovskites.Our findings provide new insights into the mixed-cation alloying strategies for improved photocatalytic performance of Pb-free perovskites and shed light on the rational design of robust band structure toward efficient energy transfer.展开更多
Lead-based organic-inorganic hybrid perovskites have exhibited great potential in photovoltaics,achieving power conversion efficiencies(PCEs) exceeding 25%.However,the toxicity of lead and the instability of these mat...Lead-based organic-inorganic hybrid perovskites have exhibited great potential in photovoltaics,achieving power conversion efficiencies(PCEs) exceeding 25%.However,the toxicity of lead and the instability of these materials under moist conditions pose significant barriers to large-scale production.To overcome these limitations,researchers have proposed mixed-valence double perovskites,where Cs_(2)Au~ⅠAu~ⅢI_6 is a particularly effective absorber due to its suitable band gap and high absorptance efficiency.To further extend the scope of these lead-free materials,we varied the trivalent gold ion and halogen anion in Cs_(2)Au~ⅠAu~ⅢI_6,resulting in 18 new structures with unique properties.Further,using first-principles calculations and elimination criteria,we identified four materials with ideal band gaps,small effective carrier mass,and strong anisotropic optical properties.According to theoretical modeling,Cs_(2)AuSbCl_6,Cs_(2)AuInCl_6,and Cs_(2)AuBiCl_6 are potential candidates for solar cell absorbers,with a spectroscopic limited maximum efficiency(SLME) of approximately 30% in a 0.25 μm-thick film.These three compounds have not been previously reported,and therefore,our work provides new insights into potential materials for solar energy conversion.We aim for this theoretical exploration of novel perovskites to guide future experiments and accelerate the development of high-performance photovoltaic devices.展开更多
The exploitation of fossil resources to meet humanity’s energy needs is the root cause of the climate warming phenomenon facing the planet. In this context, non-carbon-based energies, such as photovoltaic energy, are...The exploitation of fossil resources to meet humanity’s energy needs is the root cause of the climate warming phenomenon facing the planet. In this context, non-carbon-based energies, such as photovoltaic energy, are identified as crucial solutions. Organic perovskites MAPbI<sub>3</sub> and FAPbI<sub>3</sub>, characterized by their abundance, low cost, and ease of synthesis, are emerging as candidates for study to enhance their competitiveness. It is within this framework that this article presents a comparative analysis of the performances of MAPbI<sub>3</sub> and FAPbI<sub>3</sub> perovskites in the context of photovoltaic devices. The analysis focuses on the optoelectronic characteristics and stability of these high-potential materials. The optical properties of perovskites are rigorously evaluated, including band gaps, photoluminescence, and light absorption, using UV-Vis spectroscopy and photoluminescence techniques. The crystal structure is characterized by X-ray diffraction, while film morphology is examined through scanning electron microscopy. The results reveal significant variations between the two types of perovskites, directly impacting the performance of resulting solar devices. Simultaneously, the stability of perovskites is subjected to a thorough study, exposing the materials to various environmental conditions, highlighting key determinants of their durability. Films of MAPbI<sub>3</sub> and FAPbI<sub>3</sub> demonstrate distinct differences in terms of topography, optical performance, and stability. Research has unveiled that planar perovskite solar cells based on FAPbI<sub>3</sub> offer higher photoelectric conversion efficiency, surpassing their MAPbI<sub>3</sub>-based counterparts in terms of performance. These advancements aim to overcome stability constraints and enhance the long-term durability of perovskites, ultimately aiming for practical application of these materials. This comprehensive comparative analysis provides an enlightened understanding of the optoelectronic performance and stability of MAPbI<sub>3</sub> and FAPbI<sub>3</sub> perovskites, which is critically important to guide future research and development of solar devices that are both more efficient and sustainable.展开更多
基金Guangdong Basic and Applied Basic Research Foundation,Grant/Award Number:2023A1515012878Natural Science Foundation of Anhui Province,Grant/Award Number:2008085ME134+2 种基金Australian Research Council Discovery Projects,Grant/Award Numbers:ARC DP200103315,ARC DP200103332Major Special Science and Technology Project of Anhui Province,Grant/Award Number:202103a07020007Key Research and Development Program of Anhui Province,Grant/Award Number:202104a05020057。
文摘Ni-Fe-based oxides are among the most promising catalysts developed to date for the bottleneck oxygen evolution reaction(OER)in water electrolysis.However,understanding and mastering the synergy of Ni and Fe remain challenging.Herein,we report that the synergy between Ni and Fe can be tailored by crystal dimensionality of Ni,Fe-contained Ruddlesden-Popper(RP)-type perovskites(La_(0.125)Sr_(0.875))n+1(Ni_(0.25)Fe_(0.75))nO3n+1(n=1,2,3),where the material with n=3 shows the best OER performance in alkaline media.Soft X-ray absorption spectroscopy spectra before and after OER reveal that the material with n=3 shows enhanced Ni/Fe-O covalency to boost the electron transfer as compared to those with n=1 and n=2.Further experimental investigations demonstrate that the Fe ion is the active site and the Ni ion is the stable site in this system,where such unique synergy reaches the optimum at n=3.Besides,as n increases,the proportion of unstable rock-salt layers accordingly decreases and the leaching of ions(especially Sr^(2+))into the electrolyte is suppressed,which induces a decrease in the leaching of active Fe ions,ultimately leading to enhanced stability.This work provides a new avenue for rational catalyst design through the dimensional strategy.
基金financially supported by the National Key R&D Program of China (2022YFB4200304)the National Natural Science Foundation of China (52303347)+3 种基金the Fundamental Research Funds for the Central Universities (YJ2021157)the Engineering Featured Team Fund of Sichuan University (2020SCUNG102)open foundation of Guangxi Key Laboratory of Processing for Non-Ferrous Metals and Featured Materials, Guangxi University (2022GXYSOF05)the support from the National Natural Science Foundation of China (E30853YM19)
文摘Wide-bandgap(>1.7 eV)perovskites suffer from severe light-induced phase segregation due to high bromine content,causing irreversible damage to devices stability.However,the strategies of suppressing photoinduced phase segregation and related mechanisms have not been fully disclosed.Here,we report a new passivation agent 4-aminotetrahydrothiopyran hydrochloride(4-ATpHCl)with multifunctional groups for the interface treatment of a 1.77-eV wide-bandgap perovskite film.4-ATpH^(+)impeded halogen ion migration by anchoring on the perovskite surface,leading to the inhibition of phase segregation and thus the passivation of defects,which is ascribed to the interaction of 4-ATpH^(+)with perovskite and the formation of low-dimensional perovskites.Finally,the champion device achieved an efficiency of 19.32%with an open-circuit voltage(V_(OC))of 1.314 V and a fill factor of 83.32%.Moreover,4-ATpHCl modified device exhibited significant improved stability as compared with control one.The target device maintained 80%of its initial efficiency after 519 h of maximum power output(MPP)tracking under 1 sun illumination,however,the control device showed a rapid decrease in efficiency after 267 h.Finally,an efficiency of 27.38%of the champion 4-terminal all-perovskite tandem solar cell was achieved by mechanically stacking this wide-bandgap top subcell with a 1.25-eV low-bandgap perovskite bottom subcell.
文摘Energy supply dominated by fossil energy has been and remains the main cause of carbon dioxide emissions,the major greenhouse gas leading to the current grave climate change challenges.Many technical pathways have been proposed to address the challenges.Carbon capture and utilization(CCU) represents one of the approaches and thermochemical CO_(2) splitting driven by thermal energy is a subset of the CCU,which converts the captured CO_(2) into CO and makes it possible to achieve closed-loop carbon recirculation.Redox-active catalysts are among the most critical components of the thermochemical splitting cycles and perovskites are regarded as the most promising catalysts.Here we review the latest advancements in thermochemical cycles based on perovskites,covering thermodynamic principles,material modifications,reaction kinetics,oxygen pressure control,circular strategies,and demonstrations to provide a comprehensive overview of the topical area.Thermochemical cycles based on such materials require the consideration of trade-off between cost and efficiency,which is related to actual material used,operation mode,oxygen removal,and heat recovery.Lots of efforts have been made towards improving reaction rates,conversion efficiency and cycling stability,materials related research has been lacking-a key aspect affecting the performance across all above aspects.Double perovskites and composite perovskites arise recently as a potentially promising addition to material candidates.For such materials,more effective oxygen removal would be needed to enhance the overall efficiency,for which thermochemical or electrochemical oxygen pumps could contribute to efficient oxygen removal as well as serve as means for inert gas regeneration.The integration of thermochemical CO_(2) splitting process with downstream fuel production and other processes could reduce costs and increase efficiency of the technology.This represents one of the directions for the future research.
基金financially supported by the National Natural Science Foundation of China(52330004)the Fundamental Research Funds for the Central Universities(WUT:2023IVA075 and 2023IVB009)+3 种基金the financial support from RISE project Grant(Q-CDBK)Start-up Fund for RAPs under the Strategic Hiring Scheme(PoluU)(1-BD1H)PRI Strategic Grant(1-CD7X)RI-iWEAR Strategic Supporting Scheme(1-CD94)。
文摘Wide-bandgap(WBG)perovskite solar cells(PSCs)play a fundamental role in perovskite-based tandem solar cells.However,the efficiency of WBG PSCs is limited by significant open-circuit voltage losses,which are primarily caused by surface defects.In this study,we present a novel method for modifying surfaces using the multifunctional S-ethylisothiourea hydrobromide(SEBr),which can passivate both Pb^(-1)and FA^(-1)terminated surfaces,Moreover,the SEBr upshifted the Fermi level at the perovskite interface,thereby promoting carrier collection.This proposed method was effective for both 1.67 and 1.77 eV WBG PSCs,achieving power conversion efficiencies(PCEs)of 22.47%and 19.90%,respectively,with V_(OC)values of 1.28 and 1.33 V,along with improved film and device stability.With this advancement,we were able to fabricate monolithic all-perovskite tandem solar cells with a champion PCE of 27.10%,This research offers valuable insights for passivating the surface trap states of WBG perovskite through rational multifunctional molecular engineering.
基金supported by the National Key R&D Program of China(Grant No.2021YFA1400500)New Cornerstone Science Foundation through the New Cornerstone Investigator Program,and the XPLORER Prize.
文摘The next-generation hot-carrier solar cells,which can overcome the Shockley-Queisser limit by harvesting excessenergy from hot carriers,are receiving increasing attention.Lead halide perovskite(LHP)materials are considered aspromising candidates due to their exceptional photovoltaic properties,good stability and low cost.The cooling rate of hotcarriers is a key parameter influencing the performance of hot-carrier solar cells.In this work,we successfully detected hotcarrier dynamics in operando LHP devices using the two-pulse photovoltage correlation technique.To enhance the signalto-noise ratio,we applied the delay-time modulation method instead of the traditional power modulation.This advancementallowed us to detect the intraband hot carrier cooling time for the organic LHP CH_(3)NH_(3)PbBr_(3),which is as short as 0.21 ps.In comparison,the inorganic Cs-based LHP CsPbBr_(3)exhibited a longer cooling time of around 0.59 ps due to differentphonon contributions.These results provide us new insights into the optimal design of hot-carrier solar cells and highlightthe potential of LHP materials in advancing solar cell technology.
基金supported by the National Natural Science Foundation of China (U22A20142)the Fundamental Research Funds for the Central Universities (2023JC007)。
文摘CsPbI_(2)Br perovskite solar cell has been extensively studied due to its exceptional thermal stability and relatively stable perovskite phase structure.However,the presence of bromine leads to a rapid crystallization rate of CsPbI_(2)Br films,resulting in small grain size and high defect density.Additionally,CsPbI_(2)Br demonstrates poor light absorption due to its wide bandgap.Therefore,it is crucial to control the crystallization rate and increase the film thickness to reduce defect density,enhance light absorption,and improve photovoltaic performance.In this study,we utilized a PbAc_(2)-incorporated twice spincoating(PTS) process to address these issues.Initially,PbAc_(2) was added to the CsPbI_(2)Br precursor solution to form a CsPbI_(2)Br film,which was then coated with the CsPbI_(2)Br precursor solution to produce the PTS film,Ac^(-)can delay the perovskite crystallization,leading to the formation of thicker and denser CsPbI_(2)Br films.Moreover,lone-pair electrons of the oxygen atom provided by Ac^(-)formed coordination bonds with under-coordinated Pb~(2+) ions to fill halogen ion vacancies,thereby reducing the defect density.Ultimately,the PTS CsPbI_(2)Br device achieved a peak power conversion efficiency(PCE) of 16.19% and maintained 96.7% of its initial PCE over 1500 h at room temperature under 25% relative humidity without any encapsulation.
文摘The outcomes of computational study of electronic, magnetic and optical spectra for A2BX6 (A = Rb;B = Tc, Pb, Pt, Sn, W, Ir, Ta, Sb, Te, Se, Mo, Mn, Ti, Zr and X = Cl, Br) materials have been proceeded utilizing Vanderbilt Ultra Soft Pseudo Potential (US-PP) process. The Rb2PbBr6 and Rb2PbCl6 are found to be a (Г-Г) semiconductors with energy gaps of 0.275 and 1.142 eV, respectively making them promising photovoltaic materials. The metallic behavior of the materials for Rb2BX6 (B = Tc, W, Ir, Ta, Mn, Sb, Mo) has been confirmed showing the attendance of conducting lineaments. The dielectric function is found to be large close to the ultraviolet districts (3.10 - 4.13 eV). The extinction coefficient of the Rb2BX6 has the ability to be used for implements. The band structures and density of states ensure the magnetic semiconductors’ nature of the Rb2Mn (Cl, Br)6 perovskites. The total calculated magnetic moment of Rb2MnCl6 and Rb2MnB6 is 3.00μβ. Advanced spintronic technology requires room-temperature ferromagnetism. The present work confirms that, bromine and chlorine-founded double perovskites are extremely attractive for photovoltaic and optoelectronic devices.
文摘Organic-inorganic halides perovskites(OHPs)have drawn the attention of many researchers owing to their astonishing and unique optoelectronic properties.They have been extensively used for photovoltaic applications,achieving higher than 26%power conversion efficiency to date.These materials have potential to be deployed for many other applications beyond photovoltaics like photodetectors,sensors,light-emitting diodes(LEDs),and resistors.To address the looming challenge of Moore’s law and the Von Neumann bottleneck,many new technologies regarding the computation of architectures and storage of information are being extensively researched.Since the discovery of the memristor as a fourth component of the circuit,many materials are explored for memristive applications.Lately,researchers have advanced the exploration of OHPs for memristive applications.These materials possess promising memristive properties and various kinds of halide perovskites have been used for different applications that are not only limited to data storage but expand towards artificial synapses,and neuromorphic computing.Herein we summarize the recent advancements of OHPs for memristive applications,their unique electronic properties,fabrication of materials,and current progress in this field with some future perspectives and outlooks.
基金supported by the Talent Fund of Beijing Jiaotong University (No.2019RC058)the National Natural Science Foundation of China (Nos.62205013,62075009,62275013,and 12274020)。
文摘The development of tin-based devices with low toxicity is critical for the commercial viability of perovskite solar cells.However because tin halide is a stronger Lewis acid,its crystallization rate is extremely fast,resulting in the formation of numerous defects that affect the device performance of tin-based perovskite solar cells.Herein,propylamine hydrobromide(PABr)was added to the perovskite precursor solution as an additive to passivate defects and fabricate more uniform and dense perovskite films.Because propylamine cations are too large to enter the perovskite lattices,they only exist at the grain boundary to passivate surface defects and promote crystal growth in a preferred orientation.The PABr additive raises the average short-circuit current density from 19.45 to 25.47 mA·cm^(-2)by reducing carrier recombination induced by defects.Furthermore,the device’s long-term illumination stability is improved after optimization,and the hysteresis effect is negligible.The addition of PABr results in a power conversion efficiency of 9.35%.
基金the National Natural Science Foundation of China(Grant No.21975227)the Found of National defence Sci&Tech Laboratory(Grant No.6142602210306)。
文摘Energetic molecular perovskites have attracted widespread attention in the fields of energy materials due to their high detonation performance.In this work,we reported the effect of MgCo_(2)O_(4) nanosheets on the thermal decomposition of ammonium perchlorate(NH_(4)ClO_(4),AP)-based energetic molecular perovskites(AP-based energetic molecular perovskites).The morphology and structure of the MgCo_(2)O_(4) nanosheets were characterized.And their catalytic effect on the thermal decomposition of AP-based energetic molecular perovskites(H_2pz)[NH_(4)(ClO_(4))_(3)](PAP-4),(H_2dabco)[NH_(4)(ClO_(4))_(3)](DAP-4),(H_2mpz)[NH_(4)(ClO_(4))_(3)](PAP-M_(4)),and (H_2hpz)[NH_(4)(ClO_(4))_(3)](PAP-H_(4)) was analyzed.The results showed that MgCo_(2)O_(4) nanosheets had excellent intrinsically catalytic performance towards enhancing the thermal decomposition of AP-based energetic molecular perovskites.After adding MgCo_(2)O_(4) nanosheets,the thermal decomposition peak temperatures of PAP-4,DAP-4,PAP-M_(4),and PAP-H_(4) had been reduced by35.7℃,48.4℃,37.9℃,and 43.6℃,respectively.And the activation energy(Ea)of the thermal decomposition of AP-based energetic molecular perovskites had been reduced,the Eaof PAP-H_(4) decreased by 46.4 kJ/mol at most among them.The catalytic mechanism of MgCo_(2)O_(4) nanosheets for AP-based energetic molecular perovskites is analyzed.This work provides a reference for the future application of AP-based energetic molecular perovskites.
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.
文摘Hybrid lead halide perovskites have received great attention in the field of light-emitting diodes(LEDs)owing to their excellent optoelectronic properties,low cost,and high color purity.To data,the external quantum efficiency(EQE)of lead halide perovskites LEDs has been reported to exceed 20%[1].Even so,the toxicity of conventional lead has cast a gloomy shadow over their further application.
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.
基金the National Natural Science Foundation of China(Grant Nos.11674241 and 12174283)。
文摘The formation of Frohlich polarons in metal halide perovskites,arising from the charge carrier-longitudinal optical(LO)phonon coupling,has been proposed to explain their exceptional properties,but the effective identification of polarons in these materials is still a challenging task.Herein,we theoretically present the infrared optical absorption of Frohlich polarons based on the Huang-Rhys model.We find that multiphonon overtones appear as the energy of the incident photons matches the multiple LO phonons,wherein the average phonon number of a polaron can be directly evaluated by the order of the strongest overtone.These multiphonon structures sensitively depend on the scale of electronic distribution in the ground state and the dimensionality of the perovskite materials,revealing the effective modulation of competing processes between polaron formation and carrier cooling.Moreover,the order of the strongest overtone shifts to higher ones with temperature,providing a potential proof that the carrier mobility is affected by LO phonon scattering.The present model not only suggests a direct way to verify Frohlich polarons but also enriches our understanding of the properties of polarons in metal halide perovskites.
基金supported by the National Natural Science Foundation of China (No. 22279057)。
文摘Perovskite solar cells(PSCs) as a rising star in the photovoltaic field have received rapidly increasing attention recently due to the boosting power conversion efficiencies(PCEs) from 3.8% to 25.7% in the last13 years. Nevertheless, the conventional PSCs with three-dimensional(3D) halide perovskites as light absorbers suffer from inferior PCEs and poor durability under sunlight, high-temperature and humid conditions due to the high defect amount and structural instability of 3D perovskites, respectively. To tackle these crucial issues, lower-dimensional halide perovskites including zero-dimensional(0D), onedimensional(1D), and two-dimensional(2D) perovskites have been employed as efficient passivators to boost the PCEs and durability of 3D-PSCs due to the high structural stability and superior resistance against moisture, heat and sunlight. Therefore, in order to achieve better understanding about the advantages and superiorities of combining low-dimensional perovskites with their 3D counterparts in improving the PCEs and durability of 3D-PSCs, the recent advances in the development and fabrication of mixeddimensional PSCs with 1D/0D perovskites as passivators are summarized and discussed in the review.The superiority of 1D/0D perovskites as passivators over 2D counterparts, the passivation mechanism and the methods of 1D/0D perovskites are also presented and discussed. Furthermore, the rules to choose1D/0D perovskites or relevant spacer cations are also emphasized. On this basis, several specific strategies to design and fabricate mixed-dimensional PSCs with 1D/0D perovskites are presented and discussed.Finally, the crucial challenges and future research directions of mixed-dimensional PSCs with 1D/0D perovskites as passivators are also proposed and discussed. This review will provide some useful insights for the future development of high-efficiency and durable mixed-dimensional PSCs.
基金supported by the National High Technology Research and Development Program(2015AA050601)the National Natural Science Foundation of China(61904126,12134010,12174290)。
文摘Wide-bandgap(WBG)perovskites have been attracting much attention because of their immense potential as a front light-absorber for tandem solar cells.However,WBG perovskite solar cells(PSCs)generally exhibit undesired large open-circuit voltage(VOC)loss due to light-induced phase segregation and severe non-radiative recombination loss.Herein,antimony potassium tartrate(APTA)is added to perovskite precursor as a multifunctional additive that not only coordinates with unbonded lead but also inhibits the migration of halogen in perovskite,which results in suppressed non-radiative recombination,inhibited phase segregation and better band energy alignment.Therefore,a APTA auxiliary WBG PSC with a champion photoelectric conversion efficiency of 20.35%and less hysteresis is presented.They maintain 80%of their initial efficiencies under 100 mW cm^(-2)white light illumination in nitrogen after 1,000 h.Furthermore,by combining a semi-transparent WBG perovskite front cell with a narrow-bandgap tin–lead PSC,a perovskite/perovskite four-terminal tandem solar cell with an efficiency over 26%is achieved.Our work provides a feasible approach for the fabrication of efficient tandem solar cells.
基金financially supported by the National Natural Science Foundation of China(22179072,22002070)the Natural Science Foundation of Shandong Province(ZR2021QF006)+3 种基金the Outstanding Youth Science Foundation of Shandong Province(Overseas)(2022HWYQ-006)the Natural Science Foundation of Shandong Province(ZR2020QB059)the Fundamental Research Center of Artificial Photosynthesis(FReCAP)financially supported by the National Natural Science Foundation of China(22088102)the China Postdoctoral Science Foundation(No.2022M711898)。
文摘Lead(Pb)-free halide perovskites have recently attracted increasing attention as potential catalysts for CO_(2) photoreduction to CO due to their potential to capture solar energy and drive catalytic reaction.However,issues of the poor charge transfer still remain one of the main obstacles limiting their performance due to the overwhelming radiative and nonradiative charge-carrier recombination losses.Herein,Pb-free Sb-alloyed all-inorganic quadruple perovskite Cs_(4)Mn(Bi_(1-x)Sb_(x))_(2)Cl_(12)(0≤x≤1)is synthesized as efficient photocatalyst.By Sb alloying,the undesired relaxation of photogenerated electrons from conduction band to emission centers of[MnCl6]^(4-)is greatly suppressed,resulting in a weakened PL emission and enhanced charge transfer for photocatalyst.The ensuing Cs_(4)Mn(Bi_(1-x)Sb_(x))_(2)Cl_(12) photocatalyst accomplishes efficient conversion of CO_(2)into CO,accompanied by a surprising production of H_(2)O_(2),a high valueadded product associated with water oxidation.By optimizing Sb^(3+) concentration,a high CO evolution rate of 35.1μmol g^(-1)h^(-1)is achieved,superior to most other Pb and Pb-free halide perovskites.Our findings provide new insights into the mixed-cation alloying strategies for improved photocatalytic performance of Pb-free perovskites and shed light on the rational design of robust band structure toward efficient energy transfer.
基金the National Natural Science Foundation of China (22175180, 21975260)。
文摘Lead-based organic-inorganic hybrid perovskites have exhibited great potential in photovoltaics,achieving power conversion efficiencies(PCEs) exceeding 25%.However,the toxicity of lead and the instability of these materials under moist conditions pose significant barriers to large-scale production.To overcome these limitations,researchers have proposed mixed-valence double perovskites,where Cs_(2)Au~ⅠAu~ⅢI_6 is a particularly effective absorber due to its suitable band gap and high absorptance efficiency.To further extend the scope of these lead-free materials,we varied the trivalent gold ion and halogen anion in Cs_(2)Au~ⅠAu~ⅢI_6,resulting in 18 new structures with unique properties.Further,using first-principles calculations and elimination criteria,we identified four materials with ideal band gaps,small effective carrier mass,and strong anisotropic optical properties.According to theoretical modeling,Cs_(2)AuSbCl_6,Cs_(2)AuInCl_6,and Cs_(2)AuBiCl_6 are potential candidates for solar cell absorbers,with a spectroscopic limited maximum efficiency(SLME) of approximately 30% in a 0.25 μm-thick film.These three compounds have not been previously reported,and therefore,our work provides new insights into potential materials for solar energy conversion.We aim for this theoretical exploration of novel perovskites to guide future experiments and accelerate the development of high-performance photovoltaic devices.
文摘The exploitation of fossil resources to meet humanity’s energy needs is the root cause of the climate warming phenomenon facing the planet. In this context, non-carbon-based energies, such as photovoltaic energy, are identified as crucial solutions. Organic perovskites MAPbI<sub>3</sub> and FAPbI<sub>3</sub>, characterized by their abundance, low cost, and ease of synthesis, are emerging as candidates for study to enhance their competitiveness. It is within this framework that this article presents a comparative analysis of the performances of MAPbI<sub>3</sub> and FAPbI<sub>3</sub> perovskites in the context of photovoltaic devices. The analysis focuses on the optoelectronic characteristics and stability of these high-potential materials. The optical properties of perovskites are rigorously evaluated, including band gaps, photoluminescence, and light absorption, using UV-Vis spectroscopy and photoluminescence techniques. The crystal structure is characterized by X-ray diffraction, while film morphology is examined through scanning electron microscopy. The results reveal significant variations between the two types of perovskites, directly impacting the performance of resulting solar devices. Simultaneously, the stability of perovskites is subjected to a thorough study, exposing the materials to various environmental conditions, highlighting key determinants of their durability. Films of MAPbI<sub>3</sub> and FAPbI<sub>3</sub> demonstrate distinct differences in terms of topography, optical performance, and stability. Research has unveiled that planar perovskite solar cells based on FAPbI<sub>3</sub> offer higher photoelectric conversion efficiency, surpassing their MAPbI<sub>3</sub>-based counterparts in terms of performance. These advancements aim to overcome stability constraints and enhance the long-term durability of perovskites, ultimately aiming for practical application of these materials. This comprehensive comparative analysis provides an enlightened understanding of the optoelectronic performance and stability of MAPbI<sub>3</sub> and FAPbI<sub>3</sub> perovskites, which is critically important to guide future research and development of solar devices that are both more efficient and sustainable.