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
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
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
All-inorganic perovskite solar cells(PSCs) have potential to pass the stability international standard of IEC61215:2016 but cannot deliver high performance and stability due to the poor interface contact. In this pape...All-inorganic perovskite solar cells(PSCs) have potential to pass the stability international standard of IEC61215:2016 but cannot deliver high performance and stability due to the poor interface contact. In this paper, Sn-doped TiO_(2)(Ti_(1-x)Sn_(x)O_(2)) ultrathin nanoparticles are prepared for electron transport layer(ETL) by solution process. The ultrathin Ti_(1-x)Sn_(x)O_(2) nanocrystals have greatly improved interface contact due to the facile film formation, good conductivity and high work function. The all-inorganic inverted NiOx/CsPbI_(2)Br/Ti_(1-x)Sn_(x)O_(2)p-i-n device shows a power conversion efficiency(PCE) of 14.0%. We tested the heat stability, light stability and light-heat stability. After stored in 85℃ for 65 days, the inverted PSCs still retains 98% of initial efficiency. Under continuous standard one-sun illumination for 600 h,there is no efficiency decay, and under continuous illumination at 85℃ for 200 h, the device still retains 85% of initial efficiency. The 1.0 cm^(2) device of inverted structure shows a PCE of up to 11.2%. The ultrathin Ti_(1-x)Sn_(x)O_(2)is promising to improve the scalability and stability and thus increase the commercial prospect.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
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
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
All-inorganic CsPbIBr2perovskite solar cells(PSCs)have attracted considerable research attention in recent years due to their excellent thermal stability.However,their power conversion efficiencies(PCEs)are relatively...All-inorganic CsPbIBr2perovskite solar cells(PSCs)have attracted considerable research attention in recent years due to their excellent thermal stability.However,their power conversion efficiencies(PCEs)are relatively low and still far below the theoretical limit.Here,we report the use of an organic dye molecule(namely VG1-C8)as a bifunctional interlayer between perovskite and the hole-transport layer in CsPbIBr2PSCs.Combined experimental and theoretical calculation results disclose that the multiple Lewis base sites in VG1-C8 can effectively passivate the trap states on the perovskite films.Meanwhile,theπ-conjugated dye molecule significantly accelerates the hole extraction from the perovskite absorber as evidenced by the photoluminescence analysis.Consequently,the VG1-C8 treatment simultaneously boosts the photovoltage and photocurrent density values from 1.26 V and 10.80 mA cm^(-2) to 1.31 V and 12.44 m A cm^(-2),respectively.This leads to a significant enhancement of PCE from 9.20%to12.10%under one sun irradiation(AM 1.5G).To our knowledge,this is the record efficiency reported so far for CsPbIBr_(2) PSCs.Thus,the present work demonstrates an effective interfacial passivation strategy for the development of highly efficient PSCs.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
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
Flexible wearable optoelectronic devices fabricated fromorganic–inorganic hybrid perovskites significantly accelerate the developmentof portable energy,biomedicine,and sensing fields,but their poor thermal stabilityh...Flexible wearable optoelectronic devices fabricated fromorganic–inorganic hybrid perovskites significantly accelerate the developmentof portable energy,biomedicine,and sensing fields,but their poor thermal stabilityhinders further applications.Conversely,all-inorganic perovskites possessexcellent thermal stability,but black-phase all-inorganic perovskite filmusually requires high-temperature annealing steps,which increases energy consumptionand is not conducive to the fabrication of flexible wearable devices.In this work,an unprecedented low-temperature fabrication of stable blackphaseCsPbI3perovskite films is demonstrated by the in situ hydrolysis reactionof diphenylphosphinic chloride additive.The released diphenyl phosphateand chloride ions during the hydrolysis reaction significantly lower the phasetransition temperature and effectively passivate the defects in the perovskitefilms,yielding high-performance photodetectors with a responsivity of 42.1 AW−1 and a detectivity of 1.3×10^(14)Jones.Furthermore,high-fidelity imageand photoplethysmography sensors are demonstrated based on the fabricated flexible wearable photodetectors.This work provides a newperspective for the low-temperature fabrication of large-area all-inorganic perovskite flexible optoelectronic devices.展开更多
Interface engineering has been regarded as an effective and noninvasive means to optimize the performance of perovskite solar cells(PSCs).Here,doping engineering of a ZnO electron transport layer(ETL)and CsPbI3/ZnO in...Interface engineering has been regarded as an effective and noninvasive means to optimize the performance of perovskite solar cells(PSCs).Here,doping engineering of a ZnO electron transport layer(ETL)and CsPbI3/ZnO interface engineering via introduction of an interfacial layer are employed to improve the performances of CsPbI3-based PSCs.The results show that when introducing a TiO2 buffer layer while increasing the ZnO layer doping concentration,the open-circuit voltage,power conversion efficiency,and fill factor of the CsPbI3-based PSCs can be improved to 1.31 V,21.06%,and 74.07%,respectively,which are superior to those of PSCs only modified by the TiO2 buffer layer or high-concentration doping of ZnO layer.On the one hand,the buffer layer relieves the band bending and structural disorder of CsPbI3.On the other hand,the increased doping concentration of the ZnO layer improves the conductivity of the TiO2/ZnO bilayer ETL because of the strong interaction between the TiO2 and ZnO layers.However,such phenomena are not observed for those of a PCBM/ZnO bilayer ETL because of the weak interlayer interaction of the PCBM/ZnO interface.These results provide a comprehensive understanding of the CsPbI3/ZnO interface and suggest a guideline to design high-performance PSCs.展开更多
Sluggish charge transfer in perovskite film induced by inherent defects such as uncoordinated Pb2+undoubtedly hinders the rapid response of self-powered photovoltaic-typed detector.Based on interaction between Lewis a...Sluggish charge transfer in perovskite film induced by inherent defects such as uncoordinated Pb2+undoubtedly hinders the rapid response of self-powered photovoltaic-typed detector.Based on interaction between Lewis acids and bases,herein,we employ thiourea molecule as a multifunctional Lewis base to significantly improve the quality of all-inorganic CsPbIBr2 perovskite film.After careful characterizations,the quality of perovskite film has been well regulated.Arising from the reduced defect and the reinforced the interfacial charge extraction owing to the strong interaction between uncoordinated Pb2+ions and the-C=S groups in thiourea and the formation of hydrogen bond at perovskite/TiO_(2) interface,an enhanced responsivity of 0.335 A W-1 and specific detectivity of 3.92×10^(12) Jones has been achieved for the self-powered,carbon-electrode based photodetector,which is comparable to the state-of-theart device based on CsPbIBr2 film.More importantly,the device free of encapsulation remains 82.8%of initial performance after storage over 56 days in ambient atmosphere,promoting the practical deployment of perovskite products.展开更多
The newly emerging metal halide perovskites have attracted considerable attention due to their exceptional optoelectronic properties. This upsurge was initially driven when the power conversion efficiency of perovskit...The newly emerging metal halide perovskites have attracted considerable attention due to their exceptional optoelectronic properties. This upsurge was initially driven when the power conversion efficiency of perovskite-based photovoltaic devices exceeded 23%. Due to their optoelectronic properties, perovskite materials have also been used in light-emitting diodes, photodetectors, lasers, and memory devices. This study comprehensively discusses the recent progress of allinorganic perovskite-based photodetectors, focusing on their structures, morphologies of their constituent materials, and diverse device architectures that improve the performance metrics of these photodetectors. A brief outlook, highlighting the main existing problems, possible solutions to these problems, and future development directions, is also provided herein.展开更多
In the present investigation, we fabricated strontium (Sr2+) incorporated CsPbI2Br-based inorganic perovskite solar cells in ambient conditions. The morphology, crystallinity, absorption, elemental composition and pho...In the present investigation, we fabricated strontium (Sr2+) incorporated CsPbI2Br-based inorganic perovskite solar cells in ambient conditions. The morphology, crystallinity, absorption, elemental composition and photoluminescence analysis of the bare CsPbI2Br and CsPb1-xSrxI2Br perovskite thin films were studied systematically to investigate the role of Sr2+ incorporation. It is observed that the surface morphology of the CsPbI2Br perovskite thin film has been improved by partial substitution of Pb2+ by Sr2+ which facilitates photoactive black phase-stabilization and defect passivation. The champion device having CsPb0.98Sr0.02I2Br composition exhibited a power conversion efficiency (PCE) of 16.61% which is much higher than the bare device (13.65%). Furthermore, our CsPb0.98Sr0.02I2Br-based devices maintain > 85% of its initial efficiency over 100 h in ambient conditions.展开更多
The photovoltaic performance of perovskite sloar cells(PSCs)is strongly dependent on the crystallinity,morphorlogy and defects of perovskite films.In the present work,a novel strategy was developed to fabricate the hi...The photovoltaic performance of perovskite sloar cells(PSCs)is strongly dependent on the crystallinity,morphorlogy and defects of perovskite films.In the present work,a novel strategy was developed to fabricate the high quality CsPbI3 inorganic perovskite by tuning the growth dynamics of CsPbI3 by pretreatment of fresh CsPbI3 films with phenylethylamine iodide(PEAI).The PEAI can mediate the phase transformation from 1D(DMAPbI3)(DMA:dimethylammonium)to 3D CsPbI3 all-inorganic perovskite films via the PEA2CsPb2I7 of 2D perovskite intermediate phase,resulting in highly crystalline CsPbI3 perovskite films with remarkably enlarged grains and reduced defects.The as-achieved highly crystalline CsPbI3 inorganic perovskite not only exhibited improved phase stability but also significant reduced defects.The perovskite solar cells based on these CsPbI3 thin films exhibited a champion efficiency of 17.08%,much higher than those prepared through posttreatment or direct addition of PEAI into CsPbI3 precursor solution.This work not only developed an effective strategy to prepare high crystalline CsPbI3 film and highly efficient CsPbI3-based all-inorganic PSCs,but also unraveled the mediation mechanism of CsPbI3by pre-treatment of PEAI,shedding light for further development of high perfomance perovskite-based optoelectronics.展开更多
Cesium lead iodide(CsPbI_(3)) perovskite has gained great attention in the photovoltaic(PV) community because of its unique optoelectronic properties, good chemical stability and appropriate bandgap for sunlight harve...Cesium lead iodide(CsPbI_(3)) perovskite has gained great attention in the photovoltaic(PV) community because of its unique optoelectronic properties, good chemical stability and appropriate bandgap for sunlight harvesting applications. However, compared to solar cells fabricated from organic-inorganic hybrid perovskites, the commercialization of devices based on all-inorganic CsPbI_(3) perovskites still faces many challenges regarding PV performance and long-term stability. In this work, we discovered that tetrabutylammonium bromide(TBABr) post-treatment to CsPbI_(3) perovskite films could achieve synergistic stabilization with both TBA+cation intercalation and Br-doping. Such TBA^(+) cation intercalation leads to onedimensional capping with TBAPb I3 perovskite formed in situ, while the Br-induced crystal secondary growth helps effectively passivate the defects of CsPbI_(3) perovskite, thus enhancing the stability. In addition, the incorporation of TBABr can improve energy-level alignment and reduce interfacial charge recombination loss for better device performance. Finally, the highly stable TBABr-treated CsPbI_(3)-based perovskite solar cells show reproducible photovoltaic performance with a champion efficiency up to 19.04%, while retaining 90% of the initial efficiency after 500 h storage without encapsulation.展开更多
Adding additives into peroskite precursor solution has been proven as a simple and efficient strategy to improve the quality of peroskite films.In this work,we demonstrate an effective additive strategy to improve the...Adding additives into peroskite precursor solution has been proven as a simple and efficient strategy to improve the quality of peroskite films.In this work,we demonstrate an effective additive strategy to improve the quality of all-inorganic perovskite films by adding a novel silazane additive heptamethyldisilazane(HDMS).The power conversion efficiency(PCE)of the optimized devices is enhanced from 14.55%to 15.31%with an open-circuit voltage over 1.26 V due to the higher quality perovskite films with lower trap density after the incorporation of HDMS.More interestingly,the HDMS devices exhibit superior humidity and thermal stability compared with the control ones.This work provides a simple and efficient strategy to enhance the device performance and stability of all-inorganic perovskite solar cells,which could facilitate its commercialization.展开更多
The degradation mechanism of the all-inorganic perovskite solar cells in the ambient environment remains unclear.In this paper,water and oxygen molecule adsorptions on the all-inorganic perovskite(CsPbBr_(3))surface a...The degradation mechanism of the all-inorganic perovskite solar cells in the ambient environment remains unclear.In this paper,water and oxygen molecule adsorptions on the all-inorganic perovskite(CsPbBr_(3))surface are studied by density-functional theory calculations.In terms of the adsorption energy,the water molecules are more susceptible than the oxygen molecules to be adsorbed on the CsPbBr_(3)surface.The water molecules can be adsorbed on both the CsBr-and PbBr-terminated surfaces,but the oxygen molecules tend to be selectively adsorbed on the CsBr-terminated surface instead of the PbBr-terminated one due to the significant adsorption energy difference.While the adsorbed water molecules only contribute deep states,the oxygen molecules introduce interfacial states inside the bandgap of the perovskite,which would significantly impact the chemical and transport properties of the perovskite.Therefore,special attention should be paid to reduce the oxygen concentration in the environment during the device fabrication process so as to improve the stability and performance of the CsPbBr_(3)-based devices.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in part supported by the Start-up funds from Central Organization Department and South China University of Technologyfunds from the National Natural Science Foundation of China (U2001217)+1 种基金the Guangdong Science and Technology Program (2020B121201003, 2019ZT08L075,2019QN01L118, 2021A1515012545)the Fundamental Research Fund for the Central Universities,SCUT(2020ZYGXZR095)。
文摘All-inorganic perovskite solar cells(PSCs) have potential to pass the stability international standard of IEC61215:2016 but cannot deliver high performance and stability due to the poor interface contact. In this paper, Sn-doped TiO_(2)(Ti_(1-x)Sn_(x)O_(2)) ultrathin nanoparticles are prepared for electron transport layer(ETL) by solution process. The ultrathin Ti_(1-x)Sn_(x)O_(2) nanocrystals have greatly improved interface contact due to the facile film formation, good conductivity and high work function. The all-inorganic inverted NiOx/CsPbI_(2)Br/Ti_(1-x)Sn_(x)O_(2)p-i-n device shows a power conversion efficiency(PCE) of 14.0%. We tested the heat stability, light stability and light-heat stability. After stored in 85℃ for 65 days, the inverted PSCs still retains 98% of initial efficiency. Under continuous standard one-sun illumination for 600 h,there is no efficiency decay, and under continuous illumination at 85℃ for 200 h, the device still retains 85% of initial efficiency. The 1.0 cm^(2) device of inverted structure shows a PCE of up to 11.2%. The ultrathin Ti_(1-x)Sn_(x)O_(2)is promising to improve the scalability and stability and thus increase the commercial prospect.
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the financial support by the National Natural Science Foundation of China(52161145408 and21975038)the Fundamental Research Funds for the Central Universities(DUT20RC(3)085)。
文摘All-inorganic CsPbIBr2perovskite solar cells(PSCs)have attracted considerable research attention in recent years due to their excellent thermal stability.However,their power conversion efficiencies(PCEs)are relatively low and still far below the theoretical limit.Here,we report the use of an organic dye molecule(namely VG1-C8)as a bifunctional interlayer between perovskite and the hole-transport layer in CsPbIBr2PSCs.Combined experimental and theoretical calculation results disclose that the multiple Lewis base sites in VG1-C8 can effectively passivate the trap states on the perovskite films.Meanwhile,theπ-conjugated dye molecule significantly accelerates the hole extraction from the perovskite absorber as evidenced by the photoluminescence analysis.Consequently,the VG1-C8 treatment simultaneously boosts the photovoltage and photocurrent density values from 1.26 V and 10.80 mA cm^(-2) to 1.31 V and 12.44 m A cm^(-2),respectively.This leads to a significant enhancement of PCE from 9.20%to12.10%under one sun irradiation(AM 1.5G).To our knowledge,this is the record efficiency reported so far for CsPbIBr_(2) PSCs.Thus,the present work demonstrates an effective interfacial passivation strategy for the development of highly efficient PSCs.
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.
基金supported by the National Natural Science Foundation of China(52303257,52321006,T2394480,and T2394484)the National Key R&D Program of China(Grant No.2023YFE0111500)+3 种基金Key Research&Development and Promotion of Special Project(Scientific Problem Tackling)of Henan Province(242102211090)the China Postdoctoral Science Foundation(2023TQ0300,and 2023M743171)the Postdoctoral Fellowship Program(Grade B)of China Postdoctoral Science Foundation(GZB20230666)College Student Innovation and Entrepreneurship Training Program of Zhengzhou University(202410459200)。
文摘Flexible wearable optoelectronic devices fabricated fromorganic–inorganic hybrid perovskites significantly accelerate the developmentof portable energy,biomedicine,and sensing fields,but their poor thermal stabilityhinders further applications.Conversely,all-inorganic perovskites possessexcellent thermal stability,but black-phase all-inorganic perovskite filmusually requires high-temperature annealing steps,which increases energy consumptionand is not conducive to the fabrication of flexible wearable devices.In this work,an unprecedented low-temperature fabrication of stable blackphaseCsPbI3perovskite films is demonstrated by the in situ hydrolysis reactionof diphenylphosphinic chloride additive.The released diphenyl phosphateand chloride ions during the hydrolysis reaction significantly lower the phasetransition temperature and effectively passivate the defects in the perovskitefilms,yielding high-performance photodetectors with a responsivity of 42.1 AW−1 and a detectivity of 1.3×10^(14)Jones.Furthermore,high-fidelity imageand photoplethysmography sensors are demonstrated based on the fabricated flexible wearable photodetectors.This work provides a newperspective for the low-temperature fabrication of large-area all-inorganic perovskite flexible optoelectronic devices.
基金financially supported by the National Natural Science Foundation of China(Nos.61604119,61704131,and 61804111)Initiative Postdocs Supporting Program(No.BX20180234)+2 种基金China Postdoctoral Science Foundation(No.2018M643578)Young Elite Scientists Sponsorship Program by CAST(2016QNRC001)Fundamental Research Funds for the Central Universities.
文摘Interface engineering has been regarded as an effective and noninvasive means to optimize the performance of perovskite solar cells(PSCs).Here,doping engineering of a ZnO electron transport layer(ETL)and CsPbI3/ZnO interface engineering via introduction of an interfacial layer are employed to improve the performances of CsPbI3-based PSCs.The results show that when introducing a TiO2 buffer layer while increasing the ZnO layer doping concentration,the open-circuit voltage,power conversion efficiency,and fill factor of the CsPbI3-based PSCs can be improved to 1.31 V,21.06%,and 74.07%,respectively,which are superior to those of PSCs only modified by the TiO2 buffer layer or high-concentration doping of ZnO layer.On the one hand,the buffer layer relieves the band bending and structural disorder of CsPbI3.On the other hand,the increased doping concentration of the ZnO layer improves the conductivity of the TiO2/ZnO bilayer ETL because of the strong interaction between the TiO2 and ZnO layers.However,such phenomena are not observed for those of a PCBM/ZnO bilayer ETL because of the weak interlayer interaction of the PCBM/ZnO interface.These results provide a comprehensive understanding of the CsPbI3/ZnO interface and suggest a guideline to design high-performance PSCs.
基金supported by the National Natural Science Foundation of China(61774139,62004083,and U1802257)the Postdoctoral Research Foundation of China(2020 M683185 and 2019 M663379)+1 种基金the Fundamental Research Funds for the Central Universities(21620348,21618409 and 21619311)the Natural Science Foundation of Guangdong Province(2019B151502061,2020A1515011123)。
文摘Sluggish charge transfer in perovskite film induced by inherent defects such as uncoordinated Pb2+undoubtedly hinders the rapid response of self-powered photovoltaic-typed detector.Based on interaction between Lewis acids and bases,herein,we employ thiourea molecule as a multifunctional Lewis base to significantly improve the quality of all-inorganic CsPbIBr2 perovskite film.After careful characterizations,the quality of perovskite film has been well regulated.Arising from the reduced defect and the reinforced the interfacial charge extraction owing to the strong interaction between uncoordinated Pb2+ions and the-C=S groups in thiourea and the formation of hydrogen bond at perovskite/TiO_(2) interface,an enhanced responsivity of 0.335 A W-1 and specific detectivity of 3.92×10^(12) Jones has been achieved for the self-powered,carbon-electrode based photodetector,which is comparable to the state-of-theart device based on CsPbIBr2 film.More importantly,the device free of encapsulation remains 82.8%of initial performance after storage over 56 days in ambient atmosphere,promoting the practical deployment of perovskite products.
基金Project supported by the National Science Foundation for Distinguished Young Scholars of China(Grant No.61425021)the National Natural Science Foundation of China(Grant Nos.U1604263,11774318,and 11604302)
文摘The newly emerging metal halide perovskites have attracted considerable attention due to their exceptional optoelectronic properties. This upsurge was initially driven when the power conversion efficiency of perovskite-based photovoltaic devices exceeded 23%. Due to their optoelectronic properties, perovskite materials have also been used in light-emitting diodes, photodetectors, lasers, and memory devices. This study comprehensively discusses the recent progress of allinorganic perovskite-based photodetectors, focusing on their structures, morphologies of their constituent materials, and diverse device architectures that improve the performance metrics of these photodetectors. A brief outlook, highlighting the main existing problems, possible solutions to these problems, and future development directions, is also provided herein.
基金This work was supported by Priority Research Centre Program through the National Research Foundation of Korea(NRF)funded by the Ministry of Education,Science,and Technology(NRF-2018R1A6A1A03024334)Also,this work was supported by Priority Research Centre Program through the National Research Foundation of Korea(NRF)funded by the Ministry of Education,Science,and Technology(2020R1A2C2004880).
文摘In the present investigation, we fabricated strontium (Sr2+) incorporated CsPbI2Br-based inorganic perovskite solar cells in ambient conditions. The morphology, crystallinity, absorption, elemental composition and photoluminescence analysis of the bare CsPbI2Br and CsPb1-xSrxI2Br perovskite thin films were studied systematically to investigate the role of Sr2+ incorporation. It is observed that the surface morphology of the CsPbI2Br perovskite thin film has been improved by partial substitution of Pb2+ by Sr2+ which facilitates photoactive black phase-stabilization and defect passivation. The champion device having CsPb0.98Sr0.02I2Br composition exhibited a power conversion efficiency (PCE) of 16.61% which is much higher than the bare device (13.65%). Furthermore, our CsPb0.98Sr0.02I2Br-based devices maintain > 85% of its initial efficiency over 100 h in ambient conditions.
基金supported by the National Natural Science Foundation of China(No.51602106)。
文摘The photovoltaic performance of perovskite sloar cells(PSCs)is strongly dependent on the crystallinity,morphorlogy and defects of perovskite films.In the present work,a novel strategy was developed to fabricate the high quality CsPbI3 inorganic perovskite by tuning the growth dynamics of CsPbI3 by pretreatment of fresh CsPbI3 films with phenylethylamine iodide(PEAI).The PEAI can mediate the phase transformation from 1D(DMAPbI3)(DMA:dimethylammonium)to 3D CsPbI3 all-inorganic perovskite films via the PEA2CsPb2I7 of 2D perovskite intermediate phase,resulting in highly crystalline CsPbI3 perovskite films with remarkably enlarged grains and reduced defects.The as-achieved highly crystalline CsPbI3 inorganic perovskite not only exhibited improved phase stability but also significant reduced defects.The perovskite solar cells based on these CsPbI3 thin films exhibited a champion efficiency of 17.08%,much higher than those prepared through posttreatment or direct addition of PEAI into CsPbI3 precursor solution.This work not only developed an effective strategy to prepare high crystalline CsPbI3 film and highly efficient CsPbI3-based all-inorganic PSCs,but also unraveled the mediation mechanism of CsPbI3by pre-treatment of PEAI,shedding light for further development of high perfomance perovskite-based optoelectronics.
基金support from the National Natural Science Foundation of China (Grant Nos. 22025505, 51861145101,21777096)the Program of Shanghai Academic/Technology Research Leader (Grant No. 20XD1422200)+1 种基金the Key Laboratory of Resource Chemistry,Ministry of Education (Grant No.KLRC_ME2003)support from the Energy Materials and Surface Sciences Unit of the Okinawa Institute of Science and Technology Graduate University。
文摘Cesium lead iodide(CsPbI_(3)) perovskite has gained great attention in the photovoltaic(PV) community because of its unique optoelectronic properties, good chemical stability and appropriate bandgap for sunlight harvesting applications. However, compared to solar cells fabricated from organic-inorganic hybrid perovskites, the commercialization of devices based on all-inorganic CsPbI_(3) perovskites still faces many challenges regarding PV performance and long-term stability. In this work, we discovered that tetrabutylammonium bromide(TBABr) post-treatment to CsPbI_(3) perovskite films could achieve synergistic stabilization with both TBA+cation intercalation and Br-doping. Such TBA^(+) cation intercalation leads to onedimensional capping with TBAPb I3 perovskite formed in situ, while the Br-induced crystal secondary growth helps effectively passivate the defects of CsPbI_(3) perovskite, thus enhancing the stability. In addition, the incorporation of TBABr can improve energy-level alignment and reduce interfacial charge recombination loss for better device performance. Finally, the highly stable TBABr-treated CsPbI_(3)-based perovskite solar cells show reproducible photovoltaic performance with a champion efficiency up to 19.04%, while retaining 90% of the initial efficiency after 500 h storage without encapsulation.
基金financially supported by the National Key Research and Development Program of China(Grant No.2017YFA0206600)the National Natural Science Foundation of China(Grant No.21922505)the Strategic Priority Research Program of Chinese Academy of Sciences(Grant No.XDB36000000)。
文摘Adding additives into peroskite precursor solution has been proven as a simple and efficient strategy to improve the quality of peroskite films.In this work,we demonstrate an effective additive strategy to improve the quality of all-inorganic perovskite films by adding a novel silazane additive heptamethyldisilazane(HDMS).The power conversion efficiency(PCE)of the optimized devices is enhanced from 14.55%to 15.31%with an open-circuit voltage over 1.26 V due to the higher quality perovskite films with lower trap density after the incorporation of HDMS.More interestingly,the HDMS devices exhibit superior humidity and thermal stability compared with the control ones.This work provides a simple and efficient strategy to enhance the device performance and stability of all-inorganic perovskite solar cells,which could facilitate its commercialization.
基金supported by the Fundamental Research Funds for the Central Universities,and the National Natural Science Foundation of China(Grant Nos.91964101 and 11905016)a Project of Shandong Provincial Higher Educational Science and Technology Program(Grant No.J18KB108)+2 种基金the Fund from the State Key Laboratory of Artificial Microstructure&Mesoscopic Physicsthe Fund of the State Key Laboratory of Information Photonics and Optical Communications(Beijing University of Posts and Telecommunications)the support from the High-performance Computing Platform of Peking University。
文摘The degradation mechanism of the all-inorganic perovskite solar cells in the ambient environment remains unclear.In this paper,water and oxygen molecule adsorptions on the all-inorganic perovskite(CsPbBr_(3))surface are studied by density-functional theory calculations.In terms of the adsorption energy,the water molecules are more susceptible than the oxygen molecules to be adsorbed on the CsPbBr_(3)surface.The water molecules can be adsorbed on both the CsBr-and PbBr-terminated surfaces,but the oxygen molecules tend to be selectively adsorbed on the CsBr-terminated surface instead of the PbBr-terminated one due to the significant adsorption energy difference.While the adsorbed water molecules only contribute deep states,the oxygen molecules introduce interfacial states inside the bandgap of the perovskite,which would significantly impact the chemical and transport properties of the perovskite.Therefore,special attention should be paid to reduce the oxygen concentration in the environment during the device fabrication process so as to improve the stability and performance of the CsPbBr_(3)-based devices.
