All-inorganic CsPbIBr_(2) perovskite has attracted widespread attention in photovoltaic and other optoelectronic devices because of its superior thermal stability.However,the deposition of high-quality solutionprocess...All-inorganic CsPbIBr_(2) perovskite has attracted widespread attention in photovoltaic and other optoelectronic devices because of its superior thermal stability.However,the deposition of high-quality solutionprocessed CsPbIBr_(2) perovskite films with large thicknesses remains challenging.Here,we develop a triple-component precursor(TCP) by employing lead bromide,lead iodide,and cesium bromide,to replace the most commonly used double-component precursor(DCP) consisting of lead bromide and cesium iodide.Remarkably,the TCP system significantly increases the solution concentration to 1.3 M,leading to a larger film thickness(~390 nm) and enhanced light absorption.The resultant CsPbIBr_(2) films were evaluated in planar n-i-p structured solar cells,which exhibit a considerably higher optimal photocurrent density of 11.50 mA cm^(-2) in comparison to that of DCP-based devices(10.69 mA cm^(-2)).By adopting an organic surface passivator,the maximum device efficiency using TCP is further boosted to a record efficiency of 12.8% for CsPbIBr_(2) perovskite solar cells.展开更多
We develop the effective modification strategy based on molecular engineering of s-triazine and its derivatives to improve the photoelectric performance of all-inorganic perovskites(AIP)for the first time.The surface ...We develop the effective modification strategy based on molecular engineering of s-triazine and its derivatives to improve the photoelectric performance of all-inorganic perovskites(AIP)for the first time.The surface modification strategy with cyanuric acid successfully increases the PLQY of AIP from 40.55%to 88.15%,and significantly enhances the current of the AIP film under 3 V by almost 20-fold(from4.44 m A to 81.20 m A).This work has proven the effectiveness of improving the photoelectric performances of AIP via s-triazine and its derivatives and also suggested the potential risks of reducing the photoelectric performance of AIP due to inappropriate substituents in conjugated organic ligands.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
Facing the poor environmental stability of traditional methylammonium or formamidinium-based lead halide per-ovskites,scientists turn their attention to inorganic lead hal-ide perovskites(ILHPs)with narrow bandgaps,ex...Facing the poor environmental stability of traditional methylammonium or formamidinium-based lead halide per-ovskites,scientists turn their attention to inorganic lead hal-ide perovskites(ILHPs)with narrow bandgaps,excellent thermal stability and reduced ion migration compared to their organic/inorganic counterparts[1−4].Up to now,the PCEs for ILHP solar cells exceed 21%[5].Especially,the preferred black ILHP(e.g.CsPbI3)with the smallest bandgap of~1.7 eV and single-halide composition for avoiding phase separation is crucial for high-performance single-junction solar cells and can be applied in tandem devices as the top cells[6,7].However,small Cs+(167 pm)in CsPbI3 with a tolerance factor close to 0.8 is unsuitable for the 3D PbI3-framework[8].The mis-matched size of cations will induce lattice strain and the per-ovskite spontaneously transforms to undesired non-photoact-ive yellow phase(δ-phase,like NH4CdCl3)(Fig.1(a))[9,10].There-fore,improving lattice symmetry and reducing lattice strain are the strategies for inhibiting the phase transition of ILHPs.展开更多
Photodetectors with long detection distances and fast response are important media in constructing a non-contact human-machine interface for the Masterly Internet of Things(MIT).All-inorganic perovskites have excellen...Photodetectors with long detection distances and fast response are important media in constructing a non-contact human-machine interface for the Masterly Internet of Things(MIT).All-inorganic perovskites have excellent optoelectronic performance with high moisture and oxygen resistance,making them one of the promising candidates for high-performance photodetectors,but a simple,low-cost and reliable fabrication technology is urgently needed.Here,a dual-function laser etching method is developed to complete both the lyophilic split-ring structure and electrode patterning.This novel split-ring structure can capture the perovskite precursor droplet efficiently and achieve the uniform and compact deposition of CsPbBr3 films.Furthermore,our devices based on laterally conducting split-ring structured photodetectors possess outstanding performance,including the maximum responsivity of 1.44×105 mA W^(−1),a response time of 150μs in 1.5 kHz and one-unit area<4×10-2 mm2.Based on these split-ring photodetector arrays,we realized three-dimensional gesture detection with up to 100 mm distance detection and up to 600 mm s^(−1) speed detection,for low-cost,integrative,and non-contact human-machine interfaces.Finally,we applied this MIT to wearable and flexible digital gesture recognition watch panel,safe and comfortable central controller integrated on the car screen,and remote control of the robot,demonstrating the broad potential applications.展开更多
Doping enables manipulation of both the electrical and optical properties of halide perovskites.Herein,we incorporated Te^(4+) into Cs_(2)ZrCl_(6) single crystal,simultaneously preserving the vacancy-ordered structure...Doping enables manipulation of both the electrical and optical properties of halide perovskites.Herein,we incorporated Te^(4+) into Cs_(2)ZrCl_(6) single crystal,simultaneously preserving the vacancy-ordered structure,to obtain an efficient yellow-emitting perovskite with a near-unity photoluminescence quantum yield(PLQY≈97.6%).Te^(4+) doping modifies the hue and emission color of pristine Cs_(2)ZrCl_(6),generates new absorption channels,and successfully extends the excitation energy from<280 nm to 360-450 nm range.Detailed spectral characterizations,including ultrafast femtosecond transient absorption measurements,reveal that the bright yellow light is derived from triplet self-trapped excitons.Moreover,further tuning doping concentration enables Te-doped Cs_(2)ZrCl_(6) single crystals to exhibit efficient warm white light emission.This work provides a new perspective for the development and design of stable lead-free perovskites with highly efficient luminescence.展开更多
The emergence of perovskite solar cells(PSCs)based on all-inorganic metal halide(IMH)has generated enormous interest in the photovoltaic research community,and the power conversion efficiency(PCE)has exceeded13%.Despi...The emergence of perovskite solar cells(PSCs)based on all-inorganic metal halide(IMH)has generated enormous interest in the photovoltaic research community,and the power conversion efficiency(PCE)has exceeded13%.Despite its outstanding performance in thermal stability,PSCs based on IMH still face problems such as the lack of a suitable band gap and the inability to generate large areas.In this review,we will summarize the latest progress of PSCs based on IMH.展开更多
The energy consump tion is increasing rapidly with the continuous development of human society.Currently,global energy still mainly depends on fossil fuels.As awareness of the negative impact on the environment of bur...The energy consump tion is increasing rapidly with the continuous development of human society.Currently,global energy still mainly depends on fossil fuels.As awareness of the negative impact on the environment of burning fossil fuels,much attention has put on exploring clean and renewable energy.The solar energy has got the limitless foreground as a kind of renewable energy and photovoltaic devices can convert solar energy into electricity directly.展开更多
Metal halide perovskite nanocrystals(NCs)exhibit impressive optical and electronic properties,making them an important class of functional materials with promising applications in solar cells,light emitting diodes(LED...Metal halide perovskite nanocrystals(NCs)exhibit impressive optical and electronic properties,making them an important class of functional materials with promising applications in solar cells,light emitting diodes(LEDs),photodetectors,and photocatalysts.In addition to the widely studied 0-dimensional(0 D)metal halide perovskite NCs,such as nanocubes,low dimensional perovskites,such as 2 D all-inorganic perovskite(AIP)NCs,subsist with directionally relevant quantum confinement.These anisotropic NCs have the propensity to exhibit interesting optoelectronic properties that are exceedingly difficult to introduce into 0 D systems,yet as of late are largely unexplored.In this review,we discuss the recent synthetic progress of 2 D all-inorganic metal halide perovskite NCs with ABX3 structure.Specifically,we highlight the discrete composition control of the cations(A and B sites)and anions(X site)by dopant incorporation and alloying in 2 D metal halide perovskite NCs.We will also discuss more complex perovskite crystal structures,such as Ruddlesden-Popper double perovskites,and compare these materials to 0 D perovskite systems.Ultimately,our work culminates in the future interests and perspectives of this field with a focus on the wide applicability of 2 D systems and the large variance in structure capable with discrete compositional tuning.展开更多
Due to excellent thermal stability and optoelectronic properties, all-inorganic perovskite is one of the promising candidates to solve the thermal decomposition problem of conventional organic–inorganic hybrid perovs...Due to excellent thermal stability and optoelectronic properties, all-inorganic perovskite is one of the promising candidates to solve the thermal decomposition problem of conventional organic–inorganic hybrid perovskite solar cells(PSCs),but the larger voltage loss(V_(loss)) cannot be ignored, especially CsPbIBr_(2), which limits the improvement of efficiency. To reduce V_(loss), one promising solution is the modification of the energy level alignment between the perovskite layer and adjacent charge transport layer(CTL), which can facilitate charge extraction and reduce carrier recombination rate at the perovskite/CTL interface. Therefore, the key issues of minimum V_(loss) and high efficiency of CsPbIBr_(2)-based PSCs were studied in terms of the perovskite layer thickness, the effects of band offset of the CTL/perovskite layer, the doping concentration of the CTL, and the electrode work function in this study based on device simulations. The open-circuit voltage(V_(oc)) is increased from 1.37 V to 1.52 V by replacing SnO_(2) with ZnO as the electron transport layer(ETL) due to more matching conduction band with the CsPbIBr;layer.展开更多
All-inorganic cesium lead bromide(CsPbBr3)perovskite is attracting growing interest as functional materials in photovoltaics and other optoelectronic devices due to its superb stability.However,the fabrication of high...All-inorganic cesium lead bromide(CsPbBr3)perovskite is attracting growing interest as functional materials in photovoltaics and other optoelectronic devices due to its superb stability.However,the fabrication of high-quality CsPbBr3 films still remains a big challenge by solution-process because of the low solubility of the cesium precursor in common solvents.Herein,we report a facile solution-processed approach to prepare high-quality CsPbBr3 perovskite films via a two-step spin-coating method,in which the Cs Br methanol/H2 O mixed solvent solution is spin-coated onto the lead bromide films,followed by an isopropanol-assisted post-treatment to regulate the crystallization process and to control the film morphology.In this fashion,dense and uniform CsPbBr3 films are obtained consisting of large crystalline domains with sizes up to microns and low defect density.The effectiveness of the resulting CsPbBr3 films is further examined in perovskite solar cells(PSCs)with a simplified planar architecture of fluorine–doped tin oxide/compact Ti O2/CsPbBr3/carbon,which deliver a maximum power conversion efficiency of 8.11%together with excellent thermal and humidity stability.The present work offers a simple and effective strategy in fabrication of high-quality CsPbBr3 films for efficient and stable PSCs as well as other optoelectronic devices.展开更多
All-inorganic CsPbI_(2)Br perovskite solar cells(PSCs)have received extensive research interests recently.Nevertheless,their low efficiency and poor long-term stability are still obstacles for further commercial appli...All-inorganic CsPbI_(2)Br perovskite solar cells(PSCs)have received extensive research interests recently.Nevertheless,their low efficiency and poor long-term stability are still obstacles for further commercial application.Herein,we demonstrate that high efficiency and exceptional long-term stability are realized by incorporating gadolinium(III)chloride(GdCl_(3))into the CsPbI_(2)Br perovskite film.The incorporation of GdCl_(3) enhances the Goldschmidt tolerance factor of CsPbI_(2)Br perovskite,yielding a dense perovskite film with small grains,thus the a-phase CsPbI_(2)Br is remarkably stabilized.Additionally,it is found that the GdCl_(3)-incorporated perovskite film achieves suppressed charge recombination and appropriate energy level alignment compared with the pristine CsPbI_(2)Br film.The noticeable increment in efficiency from14.01%(control PSC)to 16.24%is achieved for GdCl_(3)-incorporated PSC.Moreover,the nonencapsulated GdCl_(3)-incorporated PSC exhibits excellent environmental and thermal stability,remaining over 91%or90%of the original efficiency after 1200 h aging at 40%relative humidity or 480 h heating at 85℃ in nitrogen glove box respectively.The encapsulated GdCl_(3)-incorporated PSC presents an improved operational stability with over 88%of initial efficiency under maximum power point(MPP)tracking at 45℃ for1000 h.This work presents an effective ion-incorporation approach for boosting efficiency and long-term stability of all-inorganic PSCs.展开更多
Tin dioxide(SnO2) is generally regarded as a promising electron-transporting layer(ETL) for state-of-theart perovskite solar cells(PSCs), however, the ubiquitous oxygen-vacancy-related defects at SnO2 surface and the ...Tin dioxide(SnO2) is generally regarded as a promising electron-transporting layer(ETL) for state-of-theart perovskite solar cells(PSCs), however, the ubiquitous oxygen-vacancy-related defects at SnO2 surface and the large energy difference between conduction band of SnO2 and perovskite layer undoubtedly cause severe charge carrier recombination, resulting in sluggish charge extraction efficiency and non-negligible open-circuit voltage(Voc) loss. Herein, a chlorine-containing TiOxCl4-2x accessory layer is fabricated by immersing SnO2 layer into the TiCl4 aqueous solution to passivate the surface oxygen-vacancy-related defects of SnO2 layer and to set an intermediate energy level at ETL/perovskite interface in all-inorganic cesium lead tri-bromine(CsPbBr3) PSCs. Furthermore, the TiOxCl4-2x layer also improves the infiltration of SnO2 layer surface toward perovskite precursor for high-quality perovskite film. Finally, the hole-free, allinorganic CsPbBr3PSC with a structure of FTO/SnO2/TiOxCl4-2x/Cs0.91Rb0.09PbBr3/carbon achieves a champion efficiency of 10.44% with a Vocas high as 1.629 V in comparison to 8.31% for control device. Moreover, the optimized solar cell presents good stability in 80% humidity in air.展开更多
A novel interface design is proposed for carbon-based,all-inorganic CsPbIBr2 perovskite solar cells(PSCs)by introducing interfacial voids between TiO2 electron transport layer and CsPbIBr2 absorber.Compared with the g...A novel interface design is proposed for carbon-based,all-inorganic CsPbIBr2 perovskite solar cells(PSCs)by introducing interfacial voids between TiO2 electron transport layer and CsPbIBr2 absorber.Compared with the general interfacial engineering strategies,this design exempts any extra modification layer in final PSC.More importantly,the interfacial voids produced by thermal decomposition of 2-phenylethylammonium iodide trigger three beneficial e ects.First,they promote the light scattering in CsPbIBr2 film and thereby boost absorption ability of the resulting CsPbIBr2 PSCs.Second,they suppress recombination of charge carriers and thus reduce dark saturation current density(J0)of the PSCs.Third,interfacial voids enlarge built-in potential(Vbi)of the PSCs,awarding increased driving force for dissociating photo-generated charge carriers.Consequently,the PSC yields the optimized e ciency of 10.20%coupled with an open-circuit voltage(Voc)of 1.338 V.The Voc achieved herein represents the best value among CsPbIBr2 PSCs reported earlier.Meanwhile,the non-encapsulated PSCs exhibit an excellent stability against light,thermal,and humidity stresses,since it remains^97%or^94%of its initial e ciency after being heated at 85℃for 12 h or stored in ambient atmosphere with relative humidity of 30–40%for 60 days,respectively.展开更多
In the past five years,all-inorganic metal halide perovskite(CsPbX3,X=Cl,Br,I)nanocrystals have been intensely studied due to their outstanding optical properties and facile synthesis,which endow them with potential o...In the past five years,all-inorganic metal halide perovskite(CsPbX3,X=Cl,Br,I)nanocrystals have been intensely studied due to their outstanding optical properties and facile synthesis,which endow them with potential optoelectronic applications.In order to optimize their physical and chemical properties,different strategies have been developed to realize the controllable synthesis of CsPbX3 nanocrystals.In this short review,we firstly present a comprehensive and detailed summary of existed synthesis strategies of CsPbX3 nanocrystals and their analogues.Then,we introduce the regulations of several reaction parameters and their effects on the morphologies of CsPbX3 nanocrystals.At the same time,we provide stability improvement methods and representative applications.Finally,we propose the current challenges and future perspectives of the promising materials.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
Light-emitting diodes based on lead halide perovskite have attracted great attention due to their outstanding performance.However,their application is plagued by the toxicity of Pb and the poor stability.Herein novel ...Light-emitting diodes based on lead halide perovskite have attracted great attention due to their outstanding performance.However,their application is plagued by the toxicity of Pb and the poor stability.Herein novel copper-based all inorganic perovskite CsCu2I3 with much enhanced stability has been reported with a potential photoluminescence quantum yield(PLQY)over 20%and self-trapped excitons(STE).By taking advantage of its extraordinary thermal stability,we successfully fabricate high-quality CsCu2I3 film through direct vacuum-based deposition(VBD)of CsCu2I3 powder.The resulting film shows almost the same PLQY with the synthesized powder,as well as excellent uniformity and stability.The perovskite light-emitting diodes(Pe-LED)based on the evaporated CsCu2I3 emitting layer achieve a luminescence of 10 cd/m2 and an external quantum efficiency(EQE)of 0.02%.To the best of our knowledge,this is the first CsCu2I3 Pe-LED fabricated by VBD with STE property,which offers a new avenue for lead-free Pe-LED.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 based on organic–inorganic hybrid perovskite materials have become a research hotspot in photovoltaics field due to their outstanding power conversion efficiency (PCE)[1]. Nonetheless, the orga...Perovskite solar cells based on organic–inorganic hybrid perovskite materials have become a research hotspot in photovoltaics field due to their outstanding power conversion efficiency (PCE)[1]. Nonetheless, the organic cations are volatile and have rotation freedom, which is not good for photoand thermal-stability of the 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
基金The authors acknowledge the financial support by the National Natural Science Foundation of China(52161145408 and 21975038)the Research and Innovation Team Project of Dalian University of Technology(DUT2022TB10)+2 种基金the Fundamental Research Funds for the Central Universities(DUT22QN213)the Innovation Technology Fund(MRP/040/21X)the Green Technology Fund(GTF202020164)for their financial support。
文摘All-inorganic CsPbIBr_(2) perovskite has attracted widespread attention in photovoltaic and other optoelectronic devices because of its superior thermal stability.However,the deposition of high-quality solutionprocessed CsPbIBr_(2) perovskite films with large thicknesses remains challenging.Here,we develop a triple-component precursor(TCP) by employing lead bromide,lead iodide,and cesium bromide,to replace the most commonly used double-component precursor(DCP) consisting of lead bromide and cesium iodide.Remarkably,the TCP system significantly increases the solution concentration to 1.3 M,leading to a larger film thickness(~390 nm) and enhanced light absorption.The resultant CsPbIBr_(2) films were evaluated in planar n-i-p structured solar cells,which exhibit a considerably higher optimal photocurrent density of 11.50 mA cm^(-2) in comparison to that of DCP-based devices(10.69 mA cm^(-2)).By adopting an organic surface passivator,the maximum device efficiency using TCP is further boosted to a record efficiency of 12.8% for CsPbIBr_(2) perovskite solar cells.
基金funded by National Natural Science Foundation of China(No.52073045)the Key Scientific and Technological Project of Jilin Province(No.20190701010GH)+2 种基金the Development and Reform Commission of Jilin Province(No.2020C0355)the support from the Key Laboratory of Nanobiosensing and Nanobioanalysis at the Universities of Jilin Provincethe support from the Jilin Provincial Department of Education。
文摘We develop the effective modification strategy based on molecular engineering of s-triazine and its derivatives to improve the photoelectric performance of all-inorganic perovskites(AIP)for the first time.The surface modification strategy with cyanuric acid successfully increases the PLQY of AIP from 40.55%to 88.15%,and significantly enhances the current of the AIP film under 3 V by almost 20-fold(from4.44 m A to 81.20 m A).This work has proven the effectiveness of improving the photoelectric performances of AIP via s-triazine and its derivatives and also suggested the potential risks of reducing the photoelectric performance of AIP due to inappropriate substituents in conjugated organic ligands.
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supported by the National Natural Science Foundation of China(62004058,U21A2076,21701041,52071048)Natural Science Foundation of Hebei Province(F2020202022)+6 种基金the Open Fund of the State Key Laboratory of Integrated Optoelectronics(IOSKL2020KF09)State Key Laboratory of Reliability and Intelligence of Electrical Equipment(EERI-PI20200005)the Support Plan for Overseas Students to Return to China for Entrepreneurship and Innovation(cx2020003)the Fundamental Research Funds for the Central Universities(2020CDJ-LHZZ-074)Natural Science Foundation of Chongqing(cstc2020jcyj-msxmX0629).L.Ding thanks the National Key Research and Development Program of China(2022YFB3803300)the open research fund of Songshan Lake Materials Laboratory(2021SLABFK02)the National Natural Science Foundation of China(21961160720).
文摘Facing the poor environmental stability of traditional methylammonium or formamidinium-based lead halide per-ovskites,scientists turn their attention to inorganic lead hal-ide perovskites(ILHPs)with narrow bandgaps,excellent thermal stability and reduced ion migration compared to their organic/inorganic counterparts[1−4].Up to now,the PCEs for ILHP solar cells exceed 21%[5].Especially,the preferred black ILHP(e.g.CsPbI3)with the smallest bandgap of~1.7 eV and single-halide composition for avoiding phase separation is crucial for high-performance single-junction solar cells and can be applied in tandem devices as the top cells[6,7].However,small Cs+(167 pm)in CsPbI3 with a tolerance factor close to 0.8 is unsuitable for the 3D PbI3-framework[8].The mis-matched size of cations will induce lattice strain and the per-ovskite spontaneously transforms to undesired non-photoact-ive yellow phase(δ-phase,like NH4CdCl3)(Fig.1(a))[9,10].There-fore,improving lattice symmetry and reducing lattice strain are the strategies for inhibiting the phase transition of ILHPs.
基金support by the Key Research Project of Zhejiang Laboratory(N.O.2021PE0AC02)the National Natural Science Foundation of China(N.O.11674210)the Project of Hetao Shenzhen-Hong Kong Science and Technology Innovation Cooperation Zone(HZQB-KCZYB-2020083).
文摘Photodetectors with long detection distances and fast response are important media in constructing a non-contact human-machine interface for the Masterly Internet of Things(MIT).All-inorganic perovskites have excellent optoelectronic performance with high moisture and oxygen resistance,making them one of the promising candidates for high-performance photodetectors,but a simple,low-cost and reliable fabrication technology is urgently needed.Here,a dual-function laser etching method is developed to complete both the lyophilic split-ring structure and electrode patterning.This novel split-ring structure can capture the perovskite precursor droplet efficiently and achieve the uniform and compact deposition of CsPbBr3 films.Furthermore,our devices based on laterally conducting split-ring structured photodetectors possess outstanding performance,including the maximum responsivity of 1.44×105 mA W^(−1),a response time of 150μs in 1.5 kHz and one-unit area<4×10-2 mm2.Based on these split-ring photodetector arrays,we realized three-dimensional gesture detection with up to 100 mm distance detection and up to 600 mm s^(−1) speed detection,for low-cost,integrative,and non-contact human-machine interfaces.Finally,we applied this MIT to wearable and flexible digital gesture recognition watch panel,safe and comfortable central controller integrated on the car screen,and remote control of the robot,demonstrating the broad potential applications.
基金supported by the National Natural Science Foundation of China (21833009, 22088102)the National Key Research and Development Program of China (2017YFA0204800)+5 种基金the Scientific Instrument Developing Project of the Chinese Academy of Sciences (YJKYYQ20190003)the Innovation Foundation of Dalian Institute of Chemical Physics (DICP I202127)the Liao Ning Revitalization Talents Program (XLYC1802126, XLYC1907053)the Dalian City Foundation for Science and Technology Innovation (2019J12GX031)the CAS Youth Innovation Promotion Association (2018220)China Postdoctoral Science Foundation (2020 M670800)。
文摘Doping enables manipulation of both the electrical and optical properties of halide perovskites.Herein,we incorporated Te^(4+) into Cs_(2)ZrCl_(6) single crystal,simultaneously preserving the vacancy-ordered structure,to obtain an efficient yellow-emitting perovskite with a near-unity photoluminescence quantum yield(PLQY≈97.6%).Te^(4+) doping modifies the hue and emission color of pristine Cs_(2)ZrCl_(6),generates new absorption channels,and successfully extends the excitation energy from<280 nm to 360-450 nm range.Detailed spectral characterizations,including ultrafast femtosecond transient absorption measurements,reveal that the bright yellow light is derived from triplet self-trapped excitons.Moreover,further tuning doping concentration enables Te-doped Cs_(2)ZrCl_(6) single crystals to exhibit efficient warm white light emission.This work provides a new perspective for the development and design of stable lead-free perovskites with highly efficient luminescence.
基金supported by the National Key R&D Program of China (Nos.2017YFA0208200,2016YFB 0700600,2015CB659300)the National Natural Science Foundation of China(Nos.21573108,51761135104)+2 种基金the Natural Science Foundation of Jiangsu Province (No. BK20150583)the High-Level Entrepreneurial and Innovative Talents Program of Jiangsu Provincethe Fundamental Research Funds for the Central Universities(No. 020514380146)
文摘The emergence of perovskite solar cells(PSCs)based on all-inorganic metal halide(IMH)has generated enormous interest in the photovoltaic research community,and the power conversion efficiency(PCE)has exceeded13%.Despite its outstanding performance in thermal stability,PSCs based on IMH still face problems such as the lack of a suitable band gap and the inability to generate large areas.In this review,we will summarize the latest progress of PSCs based on IMH.
文摘The energy consump tion is increasing rapidly with the continuous development of human society.Currently,global energy still mainly depends on fossil fuels.As awareness of the negative impact on the environment of burning fossil fuels,much attention has put on exploring clean and renewable energy.The solar energy has got the limitless foreground as a kind of renewable energy and photovoltaic devices can convert solar energy into electricity directly.
基金support from Syracuse University under the Collaboration for Unprecedented Success and Excellence(CUSE)Grant(SD-10-2020)ACS Petroleum Research Fund under Award Number 59861-DNI5NSF CAREER under Award Number CHE-1944978。
文摘Metal halide perovskite nanocrystals(NCs)exhibit impressive optical and electronic properties,making them an important class of functional materials with promising applications in solar cells,light emitting diodes(LEDs),photodetectors,and photocatalysts.In addition to the widely studied 0-dimensional(0 D)metal halide perovskite NCs,such as nanocubes,low dimensional perovskites,such as 2 D all-inorganic perovskite(AIP)NCs,subsist with directionally relevant quantum confinement.These anisotropic NCs have the propensity to exhibit interesting optoelectronic properties that are exceedingly difficult to introduce into 0 D systems,yet as of late are largely unexplored.In this review,we discuss the recent synthetic progress of 2 D all-inorganic metal halide perovskite NCs with ABX3 structure.Specifically,we highlight the discrete composition control of the cations(A and B sites)and anions(X site)by dopant incorporation and alloying in 2 D metal halide perovskite NCs.We will also discuss more complex perovskite crystal structures,such as Ruddlesden-Popper double perovskites,and compare these materials to 0 D perovskite systems.Ultimately,our work culminates in the future interests and perspectives of this field with a focus on the wide applicability of 2 D systems and the large variance in structure capable with discrete compositional tuning.
基金financially supported by the National Natural Science Foundation of China (Grant No. 52192610)the Key Research and Development Program of Shaanxi Province, China (Grant No. 2020GY-310)+2 种基金Youth Project of Natural Science Basic Research Program of Shaanxi Province, China (Grant No. 2021JQ-189)the Joint Research Funds of Department of Science & Technology of Shaanxi Province and Northwestern Polytechnical University (Grant No. 2020GXLH-Z-018)the Fundamental Research Funds for the Central Universities, China。
文摘Due to excellent thermal stability and optoelectronic properties, all-inorganic perovskite is one of the promising candidates to solve the thermal decomposition problem of conventional organic–inorganic hybrid perovskite solar cells(PSCs),but the larger voltage loss(V_(loss)) cannot be ignored, especially CsPbIBr_(2), which limits the improvement of efficiency. To reduce V_(loss), one promising solution is the modification of the energy level alignment between the perovskite layer and adjacent charge transport layer(CTL), which can facilitate charge extraction and reduce carrier recombination rate at the perovskite/CTL interface. Therefore, the key issues of minimum V_(loss) and high efficiency of CsPbIBr_(2)-based PSCs were studied in terms of the perovskite layer thickness, the effects of band offset of the CTL/perovskite layer, the doping concentration of the CTL, and the electrode work function in this study based on device simulations. The open-circuit voltage(V_(oc)) is increased from 1.37 V to 1.52 V by replacing SnO_(2) with ZnO as the electron transport layer(ETL) due to more matching conduction band with the CsPbIBr;layer.
基金financial support by the National Natural Science Foundation of China(21975038,21606039,and 51661135021)the Swiss National Science Foundation(IZLCZ2_170177)+3 种基金the Fundamental Research Funds for the Central Universities(DUT17JC39)the Swedish Foundation for Strategic Research(SSF)the Swedish Energy Agencythe Knut and Alice Wallenberg Foundation。
文摘All-inorganic cesium lead bromide(CsPbBr3)perovskite is attracting growing interest as functional materials in photovoltaics and other optoelectronic devices due to its superb stability.However,the fabrication of high-quality CsPbBr3 films still remains a big challenge by solution-process because of the low solubility of the cesium precursor in common solvents.Herein,we report a facile solution-processed approach to prepare high-quality CsPbBr3 perovskite films via a two-step spin-coating method,in which the Cs Br methanol/H2 O mixed solvent solution is spin-coated onto the lead bromide films,followed by an isopropanol-assisted post-treatment to regulate the crystallization process and to control the film morphology.In this fashion,dense and uniform CsPbBr3 films are obtained consisting of large crystalline domains with sizes up to microns and low defect density.The effectiveness of the resulting CsPbBr3 films is further examined in perovskite solar cells(PSCs)with a simplified planar architecture of fluorine–doped tin oxide/compact Ti O2/CsPbBr3/carbon,which deliver a maximum power conversion efficiency of 8.11%together with excellent thermal and humidity stability.The present work offers a simple and effective strategy in fabrication of high-quality CsPbBr3 films for efficient and stable PSCs as well as other optoelectronic devices.
基金supported by the National Natural Science Foundation of China(52172237,52072228)the Shaanxi International Cooperational Project(2020KWZ-018)+1 种基金the Research Fund of the State Key Laboratory of Solidification Processing(NPU),China(Grant No.2021-QZ-02)the Fundamental Research Funds for the Central Universities(3102019JC005)。
文摘All-inorganic CsPbI_(2)Br perovskite solar cells(PSCs)have received extensive research interests recently.Nevertheless,their low efficiency and poor long-term stability are still obstacles for further commercial application.Herein,we demonstrate that high efficiency and exceptional long-term stability are realized by incorporating gadolinium(III)chloride(GdCl_(3))into the CsPbI_(2)Br perovskite film.The incorporation of GdCl_(3) enhances the Goldschmidt tolerance factor of CsPbI_(2)Br perovskite,yielding a dense perovskite film with small grains,thus the a-phase CsPbI_(2)Br is remarkably stabilized.Additionally,it is found that the GdCl_(3)-incorporated perovskite film achieves suppressed charge recombination and appropriate energy level alignment compared with the pristine CsPbI_(2)Br film.The noticeable increment in efficiency from14.01%(control PSC)to 16.24%is achieved for GdCl_(3)-incorporated PSC.Moreover,the nonencapsulated GdCl_(3)-incorporated PSC exhibits excellent environmental and thermal stability,remaining over 91%or90%of the original efficiency after 1200 h aging at 40%relative humidity or 480 h heating at 85℃ in nitrogen glove box respectively.The encapsulated GdCl_(3)-incorporated PSC presents an improved operational stability with over 88%of initial efficiency under maximum power point(MPP)tracking at 45℃ for1000 h.This work presents an effective ion-incorporation approach for boosting efficiency and long-term stability of all-inorganic PSCs.
基金the National Natural Science Foundation of China(61774139,U1802257)Director Foundation from Qingdao National Laboratory for Marine Science and Technology(QNLM201702)+2 种基金Postdoctoral Research Foundation of China(2019M650231,2019M663379)the Natural Science Foundation of Guangdong Province(2019B151502061)the Fundamental Research Funds for the Central Universities(11618409,11619311)。
文摘Tin dioxide(SnO2) is generally regarded as a promising electron-transporting layer(ETL) for state-of-theart perovskite solar cells(PSCs), however, the ubiquitous oxygen-vacancy-related defects at SnO2 surface and the large energy difference between conduction band of SnO2 and perovskite layer undoubtedly cause severe charge carrier recombination, resulting in sluggish charge extraction efficiency and non-negligible open-circuit voltage(Voc) loss. Herein, a chlorine-containing TiOxCl4-2x accessory layer is fabricated by immersing SnO2 layer into the TiCl4 aqueous solution to passivate the surface oxygen-vacancy-related defects of SnO2 layer and to set an intermediate energy level at ETL/perovskite interface in all-inorganic cesium lead tri-bromine(CsPbBr3) PSCs. Furthermore, the TiOxCl4-2x layer also improves the infiltration of SnO2 layer surface toward perovskite precursor for high-quality perovskite film. Finally, the hole-free, allinorganic CsPbBr3PSC with a structure of FTO/SnO2/TiOxCl4-2x/Cs0.91Rb0.09PbBr3/carbon achieves a champion efficiency of 10.44% with a Vocas high as 1.629 V in comparison to 8.31% for control device. Moreover, the optimized solar cell presents good stability in 80% humidity in air.
基金financial support from the National Natural Science Foundation of China(Nos.61804113,61874083)Initiative Postdocs Supporting Program(BX20190261)+1 种基金the National Natural Science Foundation of Shaanxi Province(2018ZDCXL-GY-08-02-02 and 2017JM6049)the Fundamental Research Funds for the Central Universities(JB181107 and JBX171103).
文摘A novel interface design is proposed for carbon-based,all-inorganic CsPbIBr2 perovskite solar cells(PSCs)by introducing interfacial voids between TiO2 electron transport layer and CsPbIBr2 absorber.Compared with the general interfacial engineering strategies,this design exempts any extra modification layer in final PSC.More importantly,the interfacial voids produced by thermal decomposition of 2-phenylethylammonium iodide trigger three beneficial e ects.First,they promote the light scattering in CsPbIBr2 film and thereby boost absorption ability of the resulting CsPbIBr2 PSCs.Second,they suppress recombination of charge carriers and thus reduce dark saturation current density(J0)of the PSCs.Third,interfacial voids enlarge built-in potential(Vbi)of the PSCs,awarding increased driving force for dissociating photo-generated charge carriers.Consequently,the PSC yields the optimized e ciency of 10.20%coupled with an open-circuit voltage(Voc)of 1.338 V.The Voc achieved herein represents the best value among CsPbIBr2 PSCs reported earlier.Meanwhile,the non-encapsulated PSCs exhibit an excellent stability against light,thermal,and humidity stresses,since it remains^97%or^94%of its initial e ciency after being heated at 85℃for 12 h or stored in ambient atmosphere with relative humidity of 30–40%for 60 days,respectively.
基金supported by the Fundamental Research Funds for the Central Universities(No.2019RC020)
文摘In the past five years,all-inorganic metal halide perovskite(CsPbX3,X=Cl,Br,I)nanocrystals have been intensely studied due to their outstanding optical properties and facile synthesis,which endow them with potential optoelectronic applications.In order to optimize their physical and chemical properties,different strategies have been developed to realize the controllable synthesis of CsPbX3 nanocrystals.In this short review,we firstly present a comprehensive and detailed summary of existed synthesis strategies of CsPbX3 nanocrystals and their analogues.Then,we introduce the regulations of several reaction parameters and their effects on the morphologies of CsPbX3 nanocrystals.At the same time,we provide stability improvement methods and representative applications.Finally,we propose the current challenges and future perspectives of the promising materials.
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supported by the National Key R&D Program of China(2016YFB070700702)the National Natural Science Foundation of China(51761145048)+1 种基金the Fundamental Research Funds for the Central Universities(HUST:2019421JYCXJJ004)the China Postdoctoral Science Foundation Grant(2019M662624).
文摘Light-emitting diodes based on lead halide perovskite have attracted great attention due to their outstanding performance.However,their application is plagued by the toxicity of Pb and the poor stability.Herein novel copper-based all inorganic perovskite CsCu2I3 with much enhanced stability has been reported with a potential photoluminescence quantum yield(PLQY)over 20%and self-trapped excitons(STE).By taking advantage of its extraordinary thermal stability,we successfully fabricate high-quality CsCu2I3 film through direct vacuum-based deposition(VBD)of CsCu2I3 powder.The resulting film shows almost the same PLQY with the synthesized powder,as well as excellent uniformity and stability.The perovskite light-emitting diodes(Pe-LED)based on the evaporated CsCu2I3 emitting layer achieve a luminescence of 10 cd/m2 and an external quantum efficiency(EQE)of 0.02%.To the best of our knowledge,this is the first CsCu2I3 Pe-LED fabricated by VBD with STE property,which offers a new avenue for lead-free Pe-LED.
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 (51872321, 11874402, 52072402,51627803)the National Key Research and Development Program of China (2018YFB1500101)+1 种基金the National Key Research and Development Program of China(2017YFA0206600)the National Natural Science Foundation of China (51773045, 21772030, 51922032, 21961160720)for financial support。
文摘Perovskite solar cells based on organic–inorganic hybrid perovskite materials have become a research hotspot in photovoltaics field due to their outstanding power conversion efficiency (PCE)[1]. Nonetheless, the organic cations are volatile and have rotation freedom, which is not good for photoand thermal-stability of the 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.
