Benzoic acid containing fluorine atom at ortho-,meta-,and para-position are employed as self-assembled monolayers to modify the buried interface in perovskite solar cells(PSCs).It is demonstrated that the position of ...Benzoic acid containing fluorine atom at ortho-,meta-,and para-position are employed as self-assembled monolayers to modify the buried interface in perovskite solar cells(PSCs).It is demonstrated that the position of fluorine atom influences the passivation effect and para-fluorinated one provided the most substantial performance enhancement mainly originating from ameliorated contact and energy band alignment between NiOx and perovskite,improved perovskite quality and defect healing.Resultantly,PSC with a power conversion efficiency of 24%can be achieved.Meanwhile,which can maintain 96.8%of the initial PCE after a 1000 h storage,presenting enhanced durability.This work highlights the critical role of molecular functionality and conformation in the buried interface modification of PSCs,providing valuable insights for future developments.展开更多
As one of the important components of high-effi-ciency perovskite/silicon series devices,wide-bandgap(WBG)perovskite solar cells(PSCs)have been suffering from serious carrier transport barriers and huge open-circuit v...As one of the important components of high-effi-ciency perovskite/silicon series devices,wide-bandgap(WBG)perovskite solar cells(PSCs)have been suffering from serious carrier transport barriers and huge open-circuit voltage deficit de-rived from non-radiative recombination,especial-ly at the buried interface that are often overlooked.Herein,we combined cationic and anion passiva-tion strategies via ammonium tetra-n-butyl tetrafluoroborate(TBABF_(4))pre-treating the buried interface.Theoretical calculation predicts that the tetrabutylammonium(TBA^(+))organic cations and(tetrafluoroborate)BF_(4)^(−)anions can easily interact with charged interfacial defect.Characterizations further confirm the enhance-ment of carrier transport performance and decrease in defect density upon TBABF4 pre-treat-ment.Consequently,a power conversion efficiency of 21.35%with an ultrahigh filling factor of 84.12%is obtained for 1.68 eV-WBG inverted PSCs.In addition,the device with TBABF4 pre-treatment demonstrates excellent shelf,thermal,and operational stability.展开更多
Buried interface passivation is crucial for high-efficiency,stable perovskite solar cells(PSCs).Herein,we design a three-layer passivation structure toward the buried interface of inverted PSCs,consisting of NiO_(x),p...Buried interface passivation is crucial for high-efficiency,stable perovskite solar cells(PSCs).Herein,we design a three-layer passivation structure toward the buried interface of inverted PSCs,consisting of NiO_(x),poly(V-p-TPD)and PFN-Br(V-p-TPD,N,N'-di-p-tolyl-N,-N'-bis(4-vinylphenyl)-[1,1'-biphenyl]-4,4'-diamine;PFN-Br,poly[(9,9-bis(3'-((N,N-dimethyl)-N-ethylammonium)-propyl)-2,7-fluorene)-alt-2,7-(9,9-dioctylfluorene)]dibromide).Typically,in situ poly(V-p-TPD)layer on the NiO_(x) surface was obtained by a simple thermal crosslinking process.This poly(V-p-TPD)/NiO_(x) bilayer structure is beneficial for hole extraction and high-quality perovskite films with larger grain sizes and less lattice distortion.On this basis,the PFN-Br is further introduced as a surface modification layer,which can not only optimize the energy level alignment with the perovskite but also passivate defects and suppress carrier recombination at the perovskite bottom interface.Finally,inverted PSCs based on(FA_(0.95)Cs_(0.05))PbI_(3) present 25.5%efficiency with a low V_(OC)deficit.Besides,the devices could maintain 91.15%of the initial efficiency after being stored at 85℃for 1080 h,indicating excellent thermal stability.This work highlights the potential of a three-layered passivation structure based on crosslinking polymer HTLs for highly efficient and stable PSCs.展开更多
Numerous defects at the buried interface of perovskite film and the exacerbated oxidation and degradation of tin-lead(Sn-Pb)perovskites induced by poly(3,4-ethylenedioxythiophene):poly(styrene sulfonate)(PEDOT:PSS),du...Numerous defects at the buried interface of perovskite film and the exacerbated oxidation and degradation of tin-lead(Sn-Pb)perovskites induced by poly(3,4-ethylenedioxythiophene):poly(styrene sulfonate)(PEDOT:PSS),due to its hygroscopic and acidic nature,limit performance improvement of SnPb perovskite solar cells(PSCs).To address these issues,1-Ethyl-3-Guanidinothiourea-Hydrochloride(EGH)was employed as a multifunctional modifier at the PEDOT:PSS/perovskite interface to regulate the buried interface behaviors of Sn-Pb PSCs.EGH can not only passivate the defects of the perovskite buried interface and regulate the work function of PEDOT:PSS for a more matched interface energy level,but also prevent the perovskite film from erosion damage by the acidic PEDOT:PSS for a more stable PEDOT:PSS/perovskite interface.Moreover,the interfacial charge transport dynamics were significantly improved by obviously suppressing interfacial non-radiative recombination losses.As a consequence,EGH-tailored 1.25 eV Sn-Pb PSCs yielded a champion PCE of 23.20%,featuring enhanced long-term stability.展开更多
Interfacial defects and energy barrier would result in serious interfacial non-radiative recombination losses.In addition,the quality of perovskite films is highly dependent on deposition substrates.Consequently,there...Interfacial defects and energy barrier would result in serious interfacial non-radiative recombination losses.In addition,the quality of perovskite films is highly dependent on deposition substrates.Consequently,there is an urgent desire to develop multifunctional interface modulators to manage the interface between electron transport layer and perovskite layer.Here,we report a multifunctional buried interface modulation strategy that 4-fluoro-phenylammonium tetrafluoroborate (FBABF_(4)) consisting of simultaneously fluorinated anion and cation is inserted between SnO_(2)layer and perovskite layer.It is uncovered by time-of-flight secondary ion mass spectroscopy that the anion and cation in modifier are mainly located at this interface,which is put down to coordination bond of the fluorine atom on BF_(4)^(-) with SnO_(2),and the hydrogen bond of the fluorine atom on FBA^(+) with formamidinium.This suggests that simultaneous fluorination of anion and cation in the ionic liquid molecule is of crucial importance to ameliorate interfacial contact through chemical linker.The interface modification approach enables the realization of interfacial defect passivation,interfacial energy band alignment modulation,and perovskite crystallization manipulation,which are translated into enhanced efficiency and stability as well as significantly suppressed hysteresis.The multiple functions of FBABF_(4) endow the modified solar cells excellent photovoltaic performance with an efficiency exceeding 23%along with appealing long-term stability.This work highlights the critical role of fluorination strategy in engineering multifunctional organic salt modulators for improving interfacial contact.展开更多
For the further improvement of the power conversion efficiency(PCE)and stability of perovskite solar cells(PSCs),the buried interface between the perovskite and the electron transport layer is crucial.However,it is ch...For the further improvement of the power conversion efficiency(PCE)and stability of perovskite solar cells(PSCs),the buried interface between the perovskite and the electron transport layer is crucial.However,it is challenging to effectively optimize this interface as it is buried beneath the perovskite film.Herein,we have designed and synthesized a series of multifunctional organic-inorganic(OI)complexes as buried interfacial material to promote electron extraction,as well as the crystal growth of the perovskite.The OI complex with BF4−group not only eliminates oxygen vacancies on the SnO_(2) surface but also balances energy level alignment between SnO_(2) and perovskite,providing a favorable environment for charge carrier extraction.Moreover,OI complex with amine(−NH_(2))functional group can regulate the crystallization of the perovskite film via interaction with PbI2,resulting in highly crystallized perovskite film with large grains and low defect density.Consequently,with rational molecular design,the PSCs with optimal OI complex buried interface layer which contains both BF4−and−NH_(2) functional groups yield a champion device efficiency of 23.69%.More importantly,the resulting unencapsulated device performs excellent ambient stability,maintaining over 90%of its initial efficiency after 2000 h storage,and excellent light stability of 91.5%remaining PCE in the maximum power point tracking measurement(under continuous 100 mW cm−2 light illumination in N2 atmosphere)after 500 h.展开更多
The interfacial defects and energy barrier are main reasons for interfacial nonradiative recombination.In addition,poor perovskite crystallization and incomplete conversion of PbI_(2) to perovskite restrict further en...The interfacial defects and energy barrier are main reasons for interfacial nonradiative recombination.In addition,poor perovskite crystallization and incomplete conversion of PbI_(2) to perovskite restrict further enhancement of the photovoltaic performance of the devices using sequential deposition.Herein,a buried interface stabilization strategy that relies on the synergy of fluorine(F)and sulfonyl(S=O)functional groups is proposed.A series of potassium salts containing halide and non-halogen anions are employed to modify SnO_(2)/perovskite buried interface.Multiple chemical bonds including hydrogen bond,coordination bond and ionic bond are realized,which strengthens interfacial contact and defect passivation effect.The chemical interaction between modification molecules and perovskite along with SnO_(2) heightens incessantly as the number of S=O and F augments.The chemical interaction strength between modifiers and perovskite as well as SnO_(2) gradually increases with the increase in the number of S=O and F.The defect passivation effect is positively correlated with the chemical interaction strength.The crystallization kinetics is regulated through the compromise between chemical interaction strength and wettability of substrates.Compared with Cl−,all non-halogen anions perform better in crystallization optimization,energy band regulation and defect passivation.The device with potassium bis(fluorosulfonyl)imide achieves a tempting efficiency of 24.17%.展开更多
CsPbI_(2)Br perovskite solar cells(PSCs)have drawn tremendous attention due to their suitable bandgap,excellent photothermal stability,and great potential as an ideal candidate for top cells in tandem solar cells.Howe...CsPbI_(2)Br perovskite solar cells(PSCs)have drawn tremendous attention due to their suitable bandgap,excellent photothermal stability,and great potential as an ideal candidate for top cells in tandem solar cells.However,the abundant defects at the buried interface and perovskite layer induce severe charge recombination,resulting in the open-circuit voltage(V_(oc))output and stability much lower than anticipated.Herein,a novel buried interface management strategy is developed to regulate interfacial carrier dynamics and CsPbI_(2)Br defects by introducing ammonium tetrafluoroborate(NH_(4)BF_(4)),thereby resulting in both high CsPbI_(2)Br crystallization and minimized interfacial energy losses.Specifically,NH_(4)^(+)ions could preferentially heal hydroxyl groups on the SnO_(2)surface and balance energy level alignment between SnO_(2)and CsPbI_(2)Br,enhancing charge transport efficiency,while BF_(4)^(-)anions as a quasi-halogen regulate crystal growth of CsPbI_(2)Br,thus reducing perovskite defects.Additionally,it is proved that eliminating hydroxyl groups at the buried interface enhances the iodide migration activation energy of CsPbI_(2)Br for strengthening the phase stability.As a result,the optimized CsPbI_(2)Br PSCs realize a remarkable efficiency of 17.09%and an ultrahigh V_(oc)output of 1.43 V,which is one of the highest values for CsPbI_(2)Br PSCs.展开更多
Although ionic liquids(ILs)have been widely employed to heal the defects in perovskite solar cells(PSCs),the corresponding defect passivation mechanisms are not thoroughly understood up to now.Herein,we first reveal a...Although ionic liquids(ILs)have been widely employed to heal the defects in perovskite solar cells(PSCs),the corresponding defect passivation mechanisms are not thoroughly understood up to now.Herein,we first reveal an abnormal buried interface anion defect passivation mechanism depending on cationinduced steric hindrance.The IL molecules containing the same anion([BF4]^(-))and different sizes of imidazolium cations induced by substituent size are used to manipulate buried interface.It was revealed what passivated interfacial defects is mainly anions instead of cations.Theoretical and experimental results demonstrate that the large-sized cations can weaken the ionic bond strength between anions and cations,and facilitate the interaction between anions and SnO2as well as perovskites,which is conducive to interfacial defect passivation and ameliorating interfacial contact.It can be concluded that interfacial chemical interaction strength and defect passivation effect are positively correlated with the size of cations.The discovery breaks conventional thinking that large-sized modification molecules would weaken their chemical interaction with perovskite.Compared with the control device(21.54%),the device based on 1,3-Bis(1-adamantyl)-imidazolium tetrafluoroborate(BAIMBF4)with maximum size cations achieves a significantly enhanced efficiency of 23.61%along with much increased moisture,thermal and light stabilities.展开更多
Sum frequency generation vibrational spectroscopy(SFG-VS)is a powerful technique for determining molecular structures at both buried interface and air surface.Distinguishing the contribution of SFG signals from buried...Sum frequency generation vibrational spectroscopy(SFG-VS)is a powerful technique for determining molecular structures at both buried interface and air surface.Distinguishing the contribution of SFG signals from buried interface and air surface is crucial to the applications in devices such as microelectronics and bio-tips.Here we demonstrate that the SFG spectra from buried interface and air surface can be differentiated by controlling the film thickness and employment of surface-plasmon enhancement.Using substrate-supported PMMA(poly(methyl methacrylate))films as a model,we have visualized the variations in the contribution of SFG signals from buried interface and air surface.By monitoring carbonyl and C-H stretching groups,we found that SFG signals are dominated by the moieties(-CH2,-CH3,-OCH3 and C=O)segregated at the PMMA/air surface for the thin films while they are mainly contributed by the groups(-OCH3 and C=O)at the substrate/PMMA buried interface for the thick films.At the buried interface,the tilt angle of C=O decreases from65°to 43°as the film preparation concentration increases;in contrast,the angles at the air surface fall in the range from 38°to 21°.Surface plasmon generated by gold nanorods can largely enhance SFG signals,particularly the signals from the buried interface.展开更多
Metal halide perovskite solar cells(PSCs)are anticipated to play a pivotal role in the next generation of photovoltaic technologies,but their unsatisfactory stability hinders further commercial applications.Particular...Metal halide perovskite solar cells(PSCs)are anticipated to play a pivotal role in the next generation of photovoltaic technologies,but their unsatisfactory stability hinders further commercial applications.Particularly,numerous interfacial defects and poor mechanical adhesion at the perovskite buried interface present a critical obstacle hindering power conversion efficiency(PCE)and longterm stability of PSCs.Here,different from conventional small-molecule or linear polymer interface modifiers,we introduce a star-shaped PMMA-b-PDMAEMA(S-MD,where PMMA=poly(methyl methacrylate)and PDMAEMA=poly(dimethylaminoethyl methacrylate))polymer as a multifunctional bridge-linking polymer for simultaneous defect passivation and mechanical reinforcement at the buried interface of inverted(p-i-n)PSCs.S-MD features a three-dimensional architecture with multiple extended conjugated arms,offering multiple Lewis base functional groups(e.g.,C=O and R-N(CH_(3))_(2))with a high density of multidentate coordination sites.These groups can effectively coordinate with electron-deficient defects at the perovskite buried interface,enabling improved crystallization,reduced defect density,and enhanced interfacial adhesion.As a result,the interfacial fracture strength increases from 0.13 to 1.66 MPa.The resultant device achieves a PCE of 26.35%(certified steady-state PCE of 25.96%).The flexible device retains over 90%of its initial efficiency after 3000 flexing cycles at a curvature radius of 6 mm(R=6 mm).This work highlights a multidentate coordinating,star-shaped polymer interface strategy that offers a promising pathway toward highly efficient and stable inverted PSCs.展开更多
Buried interface defects pose a significant challenge to achieving high efficiency and stability of n-i-p perovskite solar cells(PSCs).A multifunctional material is essential for passivating interface defects,suppress...Buried interface defects pose a significant challenge to achieving high efficiency and stability of n-i-p perovskite solar cells(PSCs).A multifunctional material is essential for passivating interface defects,suppressing non-radiative recombination,and facilitating rapid carrier transfer at these interfaces.Herein,a new multifunctional eco-friendly small molecule,D-fructose,was introduced into the interface as a modification layer,playing a significant role in passivating defects not only among SnO_(2) quantum dots(QDs),but also between perovskite and SnO_(2) QDs.The coordination bonds of the C=O group with Pb^(2+)and Sn^(4+)/Sn^(2+),along with the hydrogen bonds of the-OH group with I^(-)in perovskite,contribute to this passivation process.Meanwhile,this multifunctional collaboration at the buried interface not only triggers uniform heterogeneous nucleation across the perovskite precursor film,leading to high-quality perovskite,but also effectively eliminates residual PbI2 at grain boundaries to suppress perovskite degeneration.Achieving a more suitable energy level alignment between perovskite and SnO_(2) QDs can smooth the interface barrier,thereby facilitating the formation of an electron bridge for rapid electron extraction and transfer.Consequently,the D-fructose based PSC has achieved a champion efficiency of 24.91%with negligible J-V hysteresis,along with excellent stability.展开更多
The dendrite and corrosion issues still remain for zinc anodes.Interface modification of anodes has been widely used for stabilizing zinc anodes.However,it is still quite challenging for such modification to simultane...The dendrite and corrosion issues still remain for zinc anodes.Interface modification of anodes has been widely used for stabilizing zinc anodes.However,it is still quite challenging for such modification to simultaneously suppress zinc dendrites and corrosion issues.Herein,we propose a new strategy of buried interface engineering to effectively stabilize Zn anodes,in which a zincophilic Sn layer is buried by a corrosion-resistant ZnS layer(SZS).The buried Sn layer has a strong adsorption energy towards Zn atoms,which accelerates the nucleation of Zn atoms and induces smooth deposition.Meanwhile,the outer ZnS layer protects the newly deposited zinc layer from the corrosion by the electrolyte.As a result,the SZS@Zn symmetric cell demonstrates stable cycling for over 280 h compared to Bare Zn(41 h)at a high current of 10 mA cm^(-2)and a high areal capacity of 10 mAh cm^(-2).Besides,SZS@Zn//MnO2 full cells also achieve enhanced long-term cycling stability of 63.6%for 1000 cycles at a high rate of 10 C,compared to Bare Zn(47.2%).This work provides a new strategy of buried interface for the rational design of highly stable metal anodes for other metal batteries.展开更多
In the field of perovskite solar cells(PSCs),the research on defects in the buried interface has been relatively limited due to its non-exposure;however,this interface significantly impacts the performance enhancement...In the field of perovskite solar cells(PSCs),the research on defects in the buried interface has been relatively limited due to its non-exposure;however,this interface significantly impacts the performance enhancement of inverted PSCs.This study employs phenylethylammonium chloride(PEACl)molecules as a buffer layer to modify the buried interface of p-i-n structured PSCs,aiming to enhance the uniformity of self-assembled monolayers(SAMs)and facilitate the uniform nucleation and growth of perovskite films on the substrate.Furthermore,the introduction of the PEACl buffer layer effectively passivates defects at the bottom of the perovskite layer and notably enhances the crystal quality of the perovskite film by mitigating residual stress,thereby reducing nonradiative recombination loss.Following these optimizations,the MA-free PSCs treated with PEACl achieve a power conversion efficiency(PCE)of 24.11%,with significant improvements in storage,thermal stability,and operational stability.Particularly noteworthy is the device's performance in an unencapsulated state,whereas after 1,500 hours of continuous light operation stability testing,it retains 97%of its original efficiency.This study not only enriches the systematic understanding of the characteristics of the buried interface in PSCs but also contributes significantly to advancing the commercial production of perovskite photovoltaic technology.展开更多
Wide-bandgap (WBG) flexible perovskite solarcells (pero-SCs) have aroused widespread interest because oftheir unique advantages in constructing high-efficiency tan-dems. Nickel oxide (NiO_(x)) is an excellent choice f...Wide-bandgap (WBG) flexible perovskite solarcells (pero-SCs) have aroused widespread interest because oftheir unique advantages in constructing high-efficiency tan-dems. Nickel oxide (NiO_(x)) is an excellent choice for the holetransport layer of flexible WBG pero-SCs owing to its low-temperature processing and outstanding stability. However,the presence of abundant defects at the buried perovskite layerand the weak binding force at the NiO_(x)/perovskite interfacelimit the efficiency and mechanical stability of flexible WBGpero-SCs. This study explores a buried interface modificationstrategy by introducing the functional molecule N-acetyl-L-glutamic acid (NALG) to address the above issues. Theoreticalcalculation and experimental results show that carboxyl andamide groups of NALG can bond with NiO_(x) and perovskite,respectively, which helps passivate interfacial defects and en-hances perovskite crystallization. Moreover, NALG serves as abridging molecule, significantly improving the toughness ofthe NiO_(x)/perovskite interface. Consequently, the flexible WBGpero-SC based on NiO_(x)/NALG achieved a power conversionefficiency (PCE) of 16.28% with reduced energy loss. Ad-ditionally, these flexible pero-SCs demonstrated robust me-chanical durability, retaining 83% of their initial efficienciesafter 10000 bending cycles at a radius of 5 mm. Furthermore,the devices exhibited outstanding long-term operational,thermal, and moisture stabilities.展开更多
Trap-mediated energy loss in the buried interface with non-exposed feature constitutes one of the serious challenges for achieving high-performance perovskite solar cells(PSCs).Inspired by the adhesion mechanism of mu...Trap-mediated energy loss in the buried interface with non-exposed feature constitutes one of the serious challenges for achieving high-performance perovskite solar cells(PSCs).Inspired by the adhesion mechanism of mussels,herein,three catechol derivatives with functional Lewis base groups,namely 3,4-Dihydroxyphenylalanine(DOPA),3,4-Dihydroxyphenethylamine(DA)and 3-(3,4-Dihydroxyphenyl)propionic acid(DPPA),were strategically designed.These molecules as interfacial linkers are incorporated into the buried interface between perovskite and SnO_(2) surface,achieving bilateral synergetic passivation effect.The crosslinking can produce secondary bonding with the undercoordinated Pb^(2+) and Sn^(4+) defects.The PSCs treated with DOPA exhibited the best performance and operational stability.Upon the DOPA passivation,a stabilized power conversion efficiency(PCE)of 21.5%was demonstrated for the planar PSCs.After 55 days of room-temperature storage,the unencapsulated devices with the DOPA crosslinker could still maintain 85%of their initial performance in air under relative humidity of-15%.This work opens up a new strategy for passivating the buried interfaces of perovskite photovoltaics and also provides important insights into designing defect passivation agents for other perovskite optoelectronic devices,such as light-emitting diodes,photodetectors,and lasers.展开更多
Despite the rapidly increased power conversion efficiency(PCE)of perovskite solar cells(PVSCs),it is still quite challenging to bring such promising photovoltaic technology to commercialization.One of the challenges i...Despite the rapidly increased power conversion efficiency(PCE)of perovskite solar cells(PVSCs),it is still quite challenging to bring such promising photovoltaic technology to commercialization.One of the challenges is the upscaling from small-sized lab devices to large-scale modules or panels for production.Currently,most of the efficient inverted PVSCs are fabricated on top of poly[bis(4-phenyl)(2,4,6-trimethylphenyl)amine](PTAA),which is a commonly used hole-transporting material,using spin-coating method to be incompatible with large-scale film deposition.Therefore,it is important to develop proper coating methods such as blade-coating or slot-die coating that can be compatible for producing large-area,high-quality perovskite thin films.It is found that due to the poor wettability of PTAA,the blade-coated perovskite films on PTAA surface are often inhomogeneous with large number of voids at the buried interface of the perovskite layer.To solve this problem,self-assembled monolayer(SAM)-based hole-extraction layer(HEL)with tunable headgroups on top of the SAM can be modified to provide better wettability and facilitate better interactions with the perovskite coated on top to passivate the interfacial defects.The more hydrophilic SAM surface can also facilitate the nucleation and growth of perovskite films fabricated by blade-coating methods,forming a compact and uniform buried interface.In addition,the SAM molecules can also be modified so their highest occupied molecular orbital(HOMO)levels can have a better energy alignment with the valence band maxima(VBM)of perovskite.Benefitted by the high-quality buried interface of perovskite on SAM-based substrate,the champion device shows a PCE of 18.47%and 14.64%for the devices with active areas of 0.105 cm^(2) and 1.008 cm^(2),respectively.In addition,the SAM-based device exhibits decent stability,which can maintain 90%of its initial efficiency after continuous operation for over 500 h at 40℃ in inert atmosphere.Moreover,the SAM-based perovskite mini-module exhibits a PCE of 14.13%with an aperture area of 18.0 cm^(2).This work demonstrates the great potential of using SAMs as efficient HELs for upscaling PVSCs and producing high-quality buried interface for large-area perovskite films.展开更多
Scalable deposition of high-efficiency perovskite solar cells(PSCs)is critical to accelerating their commercial applications.However,a significant number of defects are distributed at the buried interface of perovskit...Scalable deposition of high-efficiency perovskite solar cells(PSCs)is critical to accelerating their commercial applications.However,a significant number of defects are distributed at the buried interface of perovskite film fabricated by scalable deposition,exhibiting much negative influence on the efficiency and stability of PSCs.Herein,2-(N-morpholino)ethanesulfonic acid potassium salt(MESK)is incorporated as the bridging layer between the tin oxide(SnO_(2))electron transport layer(ETL)and the perovskite film deposited via scalable two-step doctor blading.Both experiment and simulation results demonstrate that MESK can passivate the trap states of Sn suspension bonds,thereby enhancing the charge extraction and transport of the SnO_(2)ETL.Meanwhile,the strong interaction with uncoordinated Pb ions can modulate the crystal growth and crystallographic orientation of perovskite film and passivate buried defects.With employing MESK interface bridging,PSCs fabricated via scalable doctor blading in ambient condition achieve a power conversion efficiency(PCE)of 24.67%,which is one of the highest PCEs for doctor-bladed PSCs,and PSC modules with an active area of 11.35 cm^(2)achieve a PCE of 19.45%.Furthermore,PSCs exhibit excellent long-term stability,and the unpackaged target device with a storage of 1680 h in ambient condition(25℃and humidity of 30%relative humidity(RH))can maintain more than 90%of the initial PCE.The research provides a strategy for constructing a high-performance interface bridge between SnO_(2)ETL and perovskite film,and achieving efficient and stable large-area PSCs and modules fabricated via scalable doctor-blading process in ambient condition.展开更多
The performance of perovskite light-emitting diodes(PeLEDs)has been drastically improved recently.Therein,the coexistence of polydisperse perovskite domains has been one worthy subject of study.The crystallization of ...The performance of perovskite light-emitting diodes(PeLEDs)has been drastically improved recently.Therein,the coexistence of polydisperse perovskite domains has been one worthy subject of study.The crystallization of perovskite is affected by the buried interface character with the bottom contact layer;and the trap states also inherently exist at the buried interface of the perovskite film,which induce the nonradiative recombination and impede the PeLED performance.In this work,we focus on the crystallization modulation of monodisperse perovskite nanodomains toward high-performance PeLEDs.We show that a LiBr pre-modification layer on the bottom substrate induces the formation of monodisperse perovskite phase.In this system,the carrier transferring process deriving from the polydisperse phases is reduced.In addition,the LiBr pre-modification layer at the buried interface minimizes the trap states and enhances the radiative recombination of perovskites.Accordingly,our PeLEDs show a champion external quantum efficiency(EQE)of 25.5%for 4 mm2 device,and 22.9%for 100 mm^(2)device.展开更多
Organic-inorganic hybrid perovskite solar cells achieve remarkable efficiencies(>26%)yet face stability challenges.Quasi-2D alternating-cation-interlayer perovskites offer enhanced stability through hydrophobic spa...Organic-inorganic hybrid perovskite solar cells achieve remarkable efficiencies(>26%)yet face stability challenges.Quasi-2D alternating-cation-interlayer perovskites offer enhanced stability through hydrophobic spacer cations but suffer from vertical phase segregation and buried interface defects.Herein,we introduce dicyanodiamide(DCD)to simultaneously address these dual limitations in GA(MA)_(n)Pb_(n)I_(3n+1)perovskites.The guanidine group in DCD passivates undercoordinated Pb^(2+)and MA^(+)vacancies at the perovskite/TiO_(2)interface,while cyano groups eliminate oxygen vacancies in TiO_(2)via Ti^(4+)-CN coordination,reducing interfacial trap density by 73%with respect to the control sample.In addition,DCD regulates crystallization kinetics,suppressing low-n-phase aggregation and promoting vertical alignment of high-n phases,which benefit for carrier transport.This dual-functional modification enhances charge transport and stabilizes energy-level alignment.The optimized devices achieve a record power conversion efficiency of 21.54%(vs.19.05%control)and retain 94%initial efficiency after 1200 h,outperforming unmodified counterparts(84%retention).Combining defect passivation with phase homogenization,this work establishes a molecular bridge strategy to decouple stability-efficiency trade-offs in low-dimensional perovskites,providing a universal framework for interface engineering in high-performance optoelectronics.展开更多
基金the Key project of Nature Science Foundation of Tianjin(22JCZDJC00120)the 111 Project(B16027)for financial support.
文摘Benzoic acid containing fluorine atom at ortho-,meta-,and para-position are employed as self-assembled monolayers to modify the buried interface in perovskite solar cells(PSCs).It is demonstrated that the position of fluorine atom influences the passivation effect and para-fluorinated one provided the most substantial performance enhancement mainly originating from ameliorated contact and energy band alignment between NiOx and perovskite,improved perovskite quality and defect healing.Resultantly,PSC with a power conversion efficiency of 24%can be achieved.Meanwhile,which can maintain 96.8%of the initial PCE after a 1000 h storage,presenting enhanced durability.This work highlights the critical role of molecular functionality and conformation in the buried interface modification of PSCs,providing valuable insights for future developments.
文摘As one of the important components of high-effi-ciency perovskite/silicon series devices,wide-bandgap(WBG)perovskite solar cells(PSCs)have been suffering from serious carrier transport barriers and huge open-circuit voltage deficit de-rived from non-radiative recombination,especial-ly at the buried interface that are often overlooked.Herein,we combined cationic and anion passiva-tion strategies via ammonium tetra-n-butyl tetrafluoroborate(TBABF_(4))pre-treating the buried interface.Theoretical calculation predicts that the tetrabutylammonium(TBA^(+))organic cations and(tetrafluoroborate)BF_(4)^(−)anions can easily interact with charged interfacial defect.Characterizations further confirm the enhance-ment of carrier transport performance and decrease in defect density upon TBABF4 pre-treat-ment.Consequently,a power conversion efficiency of 21.35%with an ultrahigh filling factor of 84.12%is obtained for 1.68 eV-WBG inverted PSCs.In addition,the device with TBABF4 pre-treatment demonstrates excellent shelf,thermal,and operational stability.
基金financial support from the Ministry of Science and Technology of China(2021YFB3800103)Natural Science Foundation of China(U24A6003,52361145847,52172260,52227803,52222212)Chinese Academy of Sciences-Commonwealth Scientific and Industrial Research Organization(CAS-CSIRO)Joint Project(112111KYSB20210017)。
文摘Buried interface passivation is crucial for high-efficiency,stable perovskite solar cells(PSCs).Herein,we design a three-layer passivation structure toward the buried interface of inverted PSCs,consisting of NiO_(x),poly(V-p-TPD)and PFN-Br(V-p-TPD,N,N'-di-p-tolyl-N,-N'-bis(4-vinylphenyl)-[1,1'-biphenyl]-4,4'-diamine;PFN-Br,poly[(9,9-bis(3'-((N,N-dimethyl)-N-ethylammonium)-propyl)-2,7-fluorene)-alt-2,7-(9,9-dioctylfluorene)]dibromide).Typically,in situ poly(V-p-TPD)layer on the NiO_(x) surface was obtained by a simple thermal crosslinking process.This poly(V-p-TPD)/NiO_(x) bilayer structure is beneficial for hole extraction and high-quality perovskite films with larger grain sizes and less lattice distortion.On this basis,the PFN-Br is further introduced as a surface modification layer,which can not only optimize the energy level alignment with the perovskite but also passivate defects and suppress carrier recombination at the perovskite bottom interface.Finally,inverted PSCs based on(FA_(0.95)Cs_(0.05))PbI_(3) present 25.5%efficiency with a low V_(OC)deficit.Besides,the devices could maintain 91.15%of the initial efficiency after being stored at 85℃for 1080 h,indicating excellent thermal stability.This work highlights the potential of a three-layered passivation structure based on crosslinking polymer HTLs for highly efficient and stable PSCs.
基金financially supported by the National Key R&D Program of China(2022YFB4200303 to D.Zhao)the National Natural Science Foundation of China(62174112,52461160298 to D.Zhao and E30853YM19 to C.Xiao)+2 种基金the Natural Science Foundation of Sichuan Province(2024NSFSC1011 to C.Chen)the Fundamental Research Funds for the Central Universities(YJ2021157 to C.Chen)the Engineering Featured Team Fund of Sichuan University(2020SCUNG102 to D.Zhao)。
文摘Numerous defects at the buried interface of perovskite film and the exacerbated oxidation and degradation of tin-lead(Sn-Pb)perovskites induced by poly(3,4-ethylenedioxythiophene):poly(styrene sulfonate)(PEDOT:PSS),due to its hygroscopic and acidic nature,limit performance improvement of SnPb perovskite solar cells(PSCs).To address these issues,1-Ethyl-3-Guanidinothiourea-Hydrochloride(EGH)was employed as a multifunctional modifier at the PEDOT:PSS/perovskite interface to regulate the buried interface behaviors of Sn-Pb PSCs.EGH can not only passivate the defects of the perovskite buried interface and regulate the work function of PEDOT:PSS for a more matched interface energy level,but also prevent the perovskite film from erosion damage by the acidic PEDOT:PSS for a more stable PEDOT:PSS/perovskite interface.Moreover,the interfacial charge transport dynamics were significantly improved by obviously suppressing interfacial non-radiative recombination losses.As a consequence,EGH-tailored 1.25 eV Sn-Pb PSCs yielded a champion PCE of 23.20%,featuring enhanced long-term stability.
基金supported by the National Natural Science Foundation of China (Grant Nos. 62004058, U21A2076, 21701041, 52071048)the Nature Science Foundation of Hebei Province (Grant No. F2020202022)+4 种基金the Open Fund of the State Key Laboratory of Integrated Optoelectronics (Grant No. IOSKL2020KF09)the State Key Laboratory of Reliability and Intelligence of Electrical Equipment (Grant No. EERI_PI20200005)supported by the Support plan for Overseas Students to Return to China for Entrepreneurship and Innovation (Grant No. cx2020003)the Fundamental Research Funds for the Central Universities (Grant No. 2020CDJ-LHZZ-074)the Natural Science Foundation of Chongqing (Grant No. cstc2020jcyjmsxmX0629)。
文摘Interfacial defects and energy barrier would result in serious interfacial non-radiative recombination losses.In addition,the quality of perovskite films is highly dependent on deposition substrates.Consequently,there is an urgent desire to develop multifunctional interface modulators to manage the interface between electron transport layer and perovskite layer.Here,we report a multifunctional buried interface modulation strategy that 4-fluoro-phenylammonium tetrafluoroborate (FBABF_(4)) consisting of simultaneously fluorinated anion and cation is inserted between SnO_(2)layer and perovskite layer.It is uncovered by time-of-flight secondary ion mass spectroscopy that the anion and cation in modifier are mainly located at this interface,which is put down to coordination bond of the fluorine atom on BF_(4)^(-) with SnO_(2),and the hydrogen bond of the fluorine atom on FBA^(+) with formamidinium.This suggests that simultaneous fluorination of anion and cation in the ionic liquid molecule is of crucial importance to ameliorate interfacial contact through chemical linker.The interface modification approach enables the realization of interfacial defect passivation,interfacial energy band alignment modulation,and perovskite crystallization manipulation,which are translated into enhanced efficiency and stability as well as significantly suppressed hysteresis.The multiple functions of FBABF_(4) endow the modified solar cells excellent photovoltaic performance with an efficiency exceeding 23%along with appealing long-term stability.This work highlights the critical role of fluorination strategy in engineering multifunctional organic salt modulators for improving interfacial contact.
基金The authors acknowledge the financial support from the Natural Science Foundation of China(Nos.21931002 and 22101123)the National Key Research and Development Program of China(2018YFB0704100)+4 种基金the Shenzhen Science and Technology Innovation Committee(no.JCYJ20200109140812302)the Leading talents of Guangdong province program(2016LJ06N507)the Guangdong Provincial Key Laboratory of Energy Materials for Electric Power(no.2018B030322001)the Guangdong Provincial Key Laboratory of Catalysis(no.2020B121201002)Outstanding Talents Training Fund in Shenzhen.
文摘For the further improvement of the power conversion efficiency(PCE)and stability of perovskite solar cells(PSCs),the buried interface between the perovskite and the electron transport layer is crucial.However,it is challenging to effectively optimize this interface as it is buried beneath the perovskite film.Herein,we have designed and synthesized a series of multifunctional organic-inorganic(OI)complexes as buried interfacial material to promote electron extraction,as well as the crystal growth of the perovskite.The OI complex with BF4−group not only eliminates oxygen vacancies on the SnO_(2) surface but also balances energy level alignment between SnO_(2) and perovskite,providing a favorable environment for charge carrier extraction.Moreover,OI complex with amine(−NH_(2))functional group can regulate the crystallization of the perovskite film via interaction with PbI2,resulting in highly crystallized perovskite film with large grains and low defect density.Consequently,with rational molecular design,the PSCs with optimal OI complex buried interface layer which contains both BF4−and−NH_(2) functional groups yield a champion device efficiency of 23.69%.More importantly,the resulting unencapsulated device performs excellent ambient stability,maintaining over 90%of its initial efficiency after 2000 h storage,and excellent light stability of 91.5%remaining PCE in the maximum power point tracking measurement(under continuous 100 mW cm−2 light illumination in N2 atmosphere)after 500 h.
基金supported by the Defense Industrial Technology Development Program(JCKY2017110C0654)National Natural Science Foundation of China(11974063,61904023,62274018)+1 种基金Chongqing Special Postdoctoral Science Foundation(cstc2019jcyj-bsh0026)Fundamental Research Funds for the Central Universities(2021CDJQY-022).
文摘The interfacial defects and energy barrier are main reasons for interfacial nonradiative recombination.In addition,poor perovskite crystallization and incomplete conversion of PbI_(2) to perovskite restrict further enhancement of the photovoltaic performance of the devices using sequential deposition.Herein,a buried interface stabilization strategy that relies on the synergy of fluorine(F)and sulfonyl(S=O)functional groups is proposed.A series of potassium salts containing halide and non-halogen anions are employed to modify SnO_(2)/perovskite buried interface.Multiple chemical bonds including hydrogen bond,coordination bond and ionic bond are realized,which strengthens interfacial contact and defect passivation effect.The chemical interaction between modification molecules and perovskite along with SnO_(2) heightens incessantly as the number of S=O and F augments.The chemical interaction strength between modifiers and perovskite as well as SnO_(2) gradually increases with the increase in the number of S=O and F.The defect passivation effect is positively correlated with the chemical interaction strength.The crystallization kinetics is regulated through the compromise between chemical interaction strength and wettability of substrates.Compared with Cl−,all non-halogen anions perform better in crystallization optimization,energy band regulation and defect passivation.The device with potassium bis(fluorosulfonyl)imide achieves a tempting efficiency of 24.17%.
基金supported by the National Natural Science Foundation of China(22379010,22109166,22309191)Chinese Academy of Sciences。
文摘CsPbI_(2)Br perovskite solar cells(PSCs)have drawn tremendous attention due to their suitable bandgap,excellent photothermal stability,and great potential as an ideal candidate for top cells in tandem solar cells.However,the abundant defects at the buried interface and perovskite layer induce severe charge recombination,resulting in the open-circuit voltage(V_(oc))output and stability much lower than anticipated.Herein,a novel buried interface management strategy is developed to regulate interfacial carrier dynamics and CsPbI_(2)Br defects by introducing ammonium tetrafluoroborate(NH_(4)BF_(4)),thereby resulting in both high CsPbI_(2)Br crystallization and minimized interfacial energy losses.Specifically,NH_(4)^(+)ions could preferentially heal hydroxyl groups on the SnO_(2)surface and balance energy level alignment between SnO_(2)and CsPbI_(2)Br,enhancing charge transport efficiency,while BF_(4)^(-)anions as a quasi-halogen regulate crystal growth of CsPbI_(2)Br,thus reducing perovskite defects.Additionally,it is proved that eliminating hydroxyl groups at the buried interface enhances the iodide migration activation energy of CsPbI_(2)Br for strengthening the phase stability.As a result,the optimized CsPbI_(2)Br PSCs realize a remarkable efficiency of 17.09%and an ultrahigh V_(oc)output of 1.43 V,which is one of the highest values for CsPbI_(2)Br PSCs.
基金financially supported by 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 and 2021CDJQY-022)Natural Science Foundation of Chongqing(cstc2020jcyjmsxmX0629)。
文摘Although ionic liquids(ILs)have been widely employed to heal the defects in perovskite solar cells(PSCs),the corresponding defect passivation mechanisms are not thoroughly understood up to now.Herein,we first reveal an abnormal buried interface anion defect passivation mechanism depending on cationinduced steric hindrance.The IL molecules containing the same anion([BF4]^(-))and different sizes of imidazolium cations induced by substituent size are used to manipulate buried interface.It was revealed what passivated interfacial defects is mainly anions instead of cations.Theoretical and experimental results demonstrate that the large-sized cations can weaken the ionic bond strength between anions and cations,and facilitate the interaction between anions and SnO2as well as perovskites,which is conducive to interfacial defect passivation and ameliorating interfacial contact.It can be concluded that interfacial chemical interaction strength and defect passivation effect are positively correlated with the size of cations.The discovery breaks conventional thinking that large-sized modification molecules would weaken their chemical interaction with perovskite.Compared with the control device(21.54%),the device based on 1,3-Bis(1-adamantyl)-imidazolium tetrafluoroborate(BAIMBF4)with maximum size cations achieves a significantly enhanced efficiency of 23.61%along with much increased moisture,thermal and light stabilities.
基金supported by the National Key Research and Development Program of China(No.2018YFA0208700 and No.2017YFA0303500)the National Natural Science Foundation of China(No.21925302,No.21633007,and No.21873090)Anhui Initiative in Quantum Information Technologies(AHY090000)。
文摘Sum frequency generation vibrational spectroscopy(SFG-VS)is a powerful technique for determining molecular structures at both buried interface and air surface.Distinguishing the contribution of SFG signals from buried interface and air surface is crucial to the applications in devices such as microelectronics and bio-tips.Here we demonstrate that the SFG spectra from buried interface and air surface can be differentiated by controlling the film thickness and employment of surface-plasmon enhancement.Using substrate-supported PMMA(poly(methyl methacrylate))films as a model,we have visualized the variations in the contribution of SFG signals from buried interface and air surface.By monitoring carbonyl and C-H stretching groups,we found that SFG signals are dominated by the moieties(-CH2,-CH3,-OCH3 and C=O)segregated at the PMMA/air surface for the thin films while they are mainly contributed by the groups(-OCH3 and C=O)at the substrate/PMMA buried interface for the thick films.At the buried interface,the tilt angle of C=O decreases from65°to 43°as the film preparation concentration increases;in contrast,the angles at the air surface fall in the range from 38°to 21°.Surface plasmon generated by gold nanorods can largely enhance SFG signals,particularly the signals from the buried interface.
基金supported by the National Natural Science Foundation of China(Nos.52125206,52433013,52273050,and 22409008)the Beijing Natural Science Foundation(No.Z240024)+3 种基金the National Key Research and Development Program of China(No.2023YFB4202502)the China Postdoctoral Science Foundation(No.2024T170023)the Qing Lan Project,the Tencent Foundation through the Xplorer Prize,the China National Petroleum Corporation-Peking University Strategic Cooperation Project of Fundamental Research,the Sinopec Seeding Programthe Yunnan Provincial Science and Technology Project at Southwest United Graduate School(No.202302AO370013).
文摘Metal halide perovskite solar cells(PSCs)are anticipated to play a pivotal role in the next generation of photovoltaic technologies,but their unsatisfactory stability hinders further commercial applications.Particularly,numerous interfacial defects and poor mechanical adhesion at the perovskite buried interface present a critical obstacle hindering power conversion efficiency(PCE)and longterm stability of PSCs.Here,different from conventional small-molecule or linear polymer interface modifiers,we introduce a star-shaped PMMA-b-PDMAEMA(S-MD,where PMMA=poly(methyl methacrylate)and PDMAEMA=poly(dimethylaminoethyl methacrylate))polymer as a multifunctional bridge-linking polymer for simultaneous defect passivation and mechanical reinforcement at the buried interface of inverted(p-i-n)PSCs.S-MD features a three-dimensional architecture with multiple extended conjugated arms,offering multiple Lewis base functional groups(e.g.,C=O and R-N(CH_(3))_(2))with a high density of multidentate coordination sites.These groups can effectively coordinate with electron-deficient defects at the perovskite buried interface,enabling improved crystallization,reduced defect density,and enhanced interfacial adhesion.As a result,the interfacial fracture strength increases from 0.13 to 1.66 MPa.The resultant device achieves a PCE of 26.35%(certified steady-state PCE of 25.96%).The flexible device retains over 90%of its initial efficiency after 3000 flexing cycles at a curvature radius of 6 mm(R=6 mm).This work highlights a multidentate coordinating,star-shaped polymer interface strategy that offers a promising pathway toward highly efficient and stable inverted PSCs.
基金supported by the Graduate Education Innovation Fund(CX2023277,CX2024082,CX2024086,CX2024097,CX2024098)of Wuhan Institute of Technologythe Natural Science Foundation of Hubei Province(2024AFB1029)。
文摘Buried interface defects pose a significant challenge to achieving high efficiency and stability of n-i-p perovskite solar cells(PSCs).A multifunctional material is essential for passivating interface defects,suppressing non-radiative recombination,and facilitating rapid carrier transfer at these interfaces.Herein,a new multifunctional eco-friendly small molecule,D-fructose,was introduced into the interface as a modification layer,playing a significant role in passivating defects not only among SnO_(2) quantum dots(QDs),but also between perovskite and SnO_(2) QDs.The coordination bonds of the C=O group with Pb^(2+)and Sn^(4+)/Sn^(2+),along with the hydrogen bonds of the-OH group with I^(-)in perovskite,contribute to this passivation process.Meanwhile,this multifunctional collaboration at the buried interface not only triggers uniform heterogeneous nucleation across the perovskite precursor film,leading to high-quality perovskite,but also effectively eliminates residual PbI2 at grain boundaries to suppress perovskite degeneration.Achieving a more suitable energy level alignment between perovskite and SnO_(2) QDs can smooth the interface barrier,thereby facilitating the formation of an electron bridge for rapid electron extraction and transfer.Consequently,the D-fructose based PSC has achieved a champion efficiency of 24.91%with negligible J-V hysteresis,along with excellent stability.
基金supported in part by the High Performance Computing Center of Central South University.We gratefully acknowledge the financial support from National Natural Science Foundation of China(52272261)The Science and Technology Innovation Program of Hunan Province(2024RC1021)+1 种基金Hunan Provincial Natural Science Foundation of China(2024JJ4062)Department of Education of Hunan Province of China(23B0020),and The Science and Technology Program of Changsha City(kq2402211).
文摘The dendrite and corrosion issues still remain for zinc anodes.Interface modification of anodes has been widely used for stabilizing zinc anodes.However,it is still quite challenging for such modification to simultaneously suppress zinc dendrites and corrosion issues.Herein,we propose a new strategy of buried interface engineering to effectively stabilize Zn anodes,in which a zincophilic Sn layer is buried by a corrosion-resistant ZnS layer(SZS).The buried Sn layer has a strong adsorption energy towards Zn atoms,which accelerates the nucleation of Zn atoms and induces smooth deposition.Meanwhile,the outer ZnS layer protects the newly deposited zinc layer from the corrosion by the electrolyte.As a result,the SZS@Zn symmetric cell demonstrates stable cycling for over 280 h compared to Bare Zn(41 h)at a high current of 10 mA cm^(-2)and a high areal capacity of 10 mAh cm^(-2).Besides,SZS@Zn//MnO2 full cells also achieve enhanced long-term cycling stability of 63.6%for 1000 cycles at a high rate of 10 C,compared to Bare Zn(47.2%).This work provides a new strategy of buried interface for the rational design of highly stable metal anodes for other metal batteries.
基金supported by the Fundamental Research Funds for the Central Universities(2024YJS192)the National Natural Science Foundation of China(62174011)。
文摘In the field of perovskite solar cells(PSCs),the research on defects in the buried interface has been relatively limited due to its non-exposure;however,this interface significantly impacts the performance enhancement of inverted PSCs.This study employs phenylethylammonium chloride(PEACl)molecules as a buffer layer to modify the buried interface of p-i-n structured PSCs,aiming to enhance the uniformity of self-assembled monolayers(SAMs)and facilitate the uniform nucleation and growth of perovskite films on the substrate.Furthermore,the introduction of the PEACl buffer layer effectively passivates defects at the bottom of the perovskite layer and notably enhances the crystal quality of the perovskite film by mitigating residual stress,thereby reducing nonradiative recombination loss.Following these optimizations,the MA-free PSCs treated with PEACl achieve a power conversion efficiency(PCE)of 24.11%,with significant improvements in storage,thermal stability,and operational stability.Particularly noteworthy is the device's performance in an unencapsulated state,whereas after 1,500 hours of continuous light operation stability testing,it retains 97%of its original efficiency.This study not only enriches the systematic understanding of the characteristics of the buried interface in PSCs but also contributes significantly to advancing the commercial production of perovskite photovoltaic technology.
基金supported by the National Key Research and Development Program of China (2024YFB4205204)the National Natural Science Foundation of China (52325307, 52473188, 22075194, 52203233, and 52273188)+3 种基金the Department of Science and Technology of Jiangsu Province (BE2022023)the Priority Academic Program Development of Jiangsu Higher Education Institutions (PAPD)the Collaborative Innovation Center of Suzhou Nano Science and Technologythe Key Laboratory of Polymeric Materials Design and Synthesis for Biomedical Function, Soochow University。
文摘Wide-bandgap (WBG) flexible perovskite solarcells (pero-SCs) have aroused widespread interest because oftheir unique advantages in constructing high-efficiency tan-dems. Nickel oxide (NiO_(x)) is an excellent choice for the holetransport layer of flexible WBG pero-SCs owing to its low-temperature processing and outstanding stability. However,the presence of abundant defects at the buried perovskite layerand the weak binding force at the NiO_(x)/perovskite interfacelimit the efficiency and mechanical stability of flexible WBGpero-SCs. This study explores a buried interface modificationstrategy by introducing the functional molecule N-acetyl-L-glutamic acid (NALG) to address the above issues. Theoreticalcalculation and experimental results show that carboxyl andamide groups of NALG can bond with NiO_(x) and perovskite,respectively, which helps passivate interfacial defects and en-hances perovskite crystallization. Moreover, NALG serves as abridging molecule, significantly improving the toughness ofthe NiO_(x)/perovskite interface. Consequently, the flexible WBGpero-SC based on NiO_(x)/NALG achieved a power conversionefficiency (PCE) of 16.28% with reduced energy loss. Ad-ditionally, these flexible pero-SCs demonstrated robust me-chanical durability, retaining 83% of their initial efficienciesafter 10000 bending cycles at a radius of 5 mm. Furthermore,the devices exhibited outstanding long-term operational,thermal, and moisture stabilities.
基金support from the National Key R&D Program of China(No.2018YFA0208501)the National Nature Science Foundation of China(Nos.51803217,51773206,91963212,and 51961145102[BRICS project])+4 种基金Beijing National Laboratory for Molecular Sciences(Nos.BNLMS-CXXM-202005 and 2019BMS20003)K.C.Wong Education Foundation,Beijing National Laboratory for Molecular Sciences(BNLMS-CXXM-202005)Key R&D and Promotion Project of Henan Province(No.192102210032)Open Project of State Key Laboratory of Silicon Materials(No.SKL2019-10)Outstanding Young Talent Research Fund of Zhengzhou University.
文摘Trap-mediated energy loss in the buried interface with non-exposed feature constitutes one of the serious challenges for achieving high-performance perovskite solar cells(PSCs).Inspired by the adhesion mechanism of mussels,herein,three catechol derivatives with functional Lewis base groups,namely 3,4-Dihydroxyphenylalanine(DOPA),3,4-Dihydroxyphenethylamine(DA)and 3-(3,4-Dihydroxyphenyl)propionic acid(DPPA),were strategically designed.These molecules as interfacial linkers are incorporated into the buried interface between perovskite and SnO_(2) surface,achieving bilateral synergetic passivation effect.The crosslinking can produce secondary bonding with the undercoordinated Pb^(2+) and Sn^(4+) defects.The PSCs treated with DOPA exhibited the best performance and operational stability.Upon the DOPA passivation,a stabilized power conversion efficiency(PCE)of 21.5%was demonstrated for the planar PSCs.After 55 days of room-temperature storage,the unencapsulated devices with the DOPA crosslinker could still maintain 85%of their initial performance in air under relative humidity of-15%.This work opens up a new strategy for passivating the buried interfaces of perovskite photovoltaics and also provides important insights into designing defect passivation agents for other perovskite optoelectronic devices,such as light-emitting diodes,photodetectors,and lasers.
基金A.K.Y.J.thanks the sponsorship of the Lee Shau-Kee Chair Professor(Materials Science),and the support from the APRC Grant of the City University of Hong Kong(No.9380086)the GRF grant(No.11307621)from the Research Grants Council of Hong Kong,Guangdong Major Project of Basic and Applied Basic Research(No.2019B030302007)Guangdong-Hong Kong-Macao Joint Laboratory of Optoelectronic and Magnetic Functional Materials(No.2019B121205002).
文摘Despite the rapidly increased power conversion efficiency(PCE)of perovskite solar cells(PVSCs),it is still quite challenging to bring such promising photovoltaic technology to commercialization.One of the challenges is the upscaling from small-sized lab devices to large-scale modules or panels for production.Currently,most of the efficient inverted PVSCs are fabricated on top of poly[bis(4-phenyl)(2,4,6-trimethylphenyl)amine](PTAA),which is a commonly used hole-transporting material,using spin-coating method to be incompatible with large-scale film deposition.Therefore,it is important to develop proper coating methods such as blade-coating or slot-die coating that can be compatible for producing large-area,high-quality perovskite thin films.It is found that due to the poor wettability of PTAA,the blade-coated perovskite films on PTAA surface are often inhomogeneous with large number of voids at the buried interface of the perovskite layer.To solve this problem,self-assembled monolayer(SAM)-based hole-extraction layer(HEL)with tunable headgroups on top of the SAM can be modified to provide better wettability and facilitate better interactions with the perovskite coated on top to passivate the interfacial defects.The more hydrophilic SAM surface can also facilitate the nucleation and growth of perovskite films fabricated by blade-coating methods,forming a compact and uniform buried interface.In addition,the SAM molecules can also be modified so their highest occupied molecular orbital(HOMO)levels can have a better energy alignment with the valence band maxima(VBM)of perovskite.Benefitted by the high-quality buried interface of perovskite on SAM-based substrate,the champion device shows a PCE of 18.47%and 14.64%for the devices with active areas of 0.105 cm^(2) and 1.008 cm^(2),respectively.In addition,the SAM-based device exhibits decent stability,which can maintain 90%of its initial efficiency after continuous operation for over 500 h at 40℃ in inert atmosphere.Moreover,the SAM-based perovskite mini-module exhibits a PCE of 14.13%with an aperture area of 18.0 cm^(2).This work demonstrates the great potential of using SAMs as efficient HELs for upscaling PVSCs and producing high-quality buried interface for large-area perovskite films.
基金support from the National Natural Science Foundation of China(No.U23A20138)the National Key Research and Development Program of China(No.2022YFB3803300).
文摘Scalable deposition of high-efficiency perovskite solar cells(PSCs)is critical to accelerating their commercial applications.However,a significant number of defects are distributed at the buried interface of perovskite film fabricated by scalable deposition,exhibiting much negative influence on the efficiency and stability of PSCs.Herein,2-(N-morpholino)ethanesulfonic acid potassium salt(MESK)is incorporated as the bridging layer between the tin oxide(SnO_(2))electron transport layer(ETL)and the perovskite film deposited via scalable two-step doctor blading.Both experiment and simulation results demonstrate that MESK can passivate the trap states of Sn suspension bonds,thereby enhancing the charge extraction and transport of the SnO_(2)ETL.Meanwhile,the strong interaction with uncoordinated Pb ions can modulate the crystal growth and crystallographic orientation of perovskite film and passivate buried defects.With employing MESK interface bridging,PSCs fabricated via scalable doctor blading in ambient condition achieve a power conversion efficiency(PCE)of 24.67%,which is one of the highest PCEs for doctor-bladed PSCs,and PSC modules with an active area of 11.35 cm^(2)achieve a PCE of 19.45%.Furthermore,PSCs exhibit excellent long-term stability,and the unpackaged target device with a storage of 1680 h in ambient condition(25℃and humidity of 30%relative humidity(RH))can maintain more than 90%of the initial PCE.The research provides a strategy for constructing a high-performance interface bridge between SnO_(2)ETL and perovskite film,and achieving efficient and stable large-area PSCs and modules fabricated via scalable doctor-blading process in ambient condition.
文摘The performance of perovskite light-emitting diodes(PeLEDs)has been drastically improved recently.Therein,the coexistence of polydisperse perovskite domains has been one worthy subject of study.The crystallization of perovskite is affected by the buried interface character with the bottom contact layer;and the trap states also inherently exist at the buried interface of the perovskite film,which induce the nonradiative recombination and impede the PeLED performance.In this work,we focus on the crystallization modulation of monodisperse perovskite nanodomains toward high-performance PeLEDs.We show that a LiBr pre-modification layer on the bottom substrate induces the formation of monodisperse perovskite phase.In this system,the carrier transferring process deriving from the polydisperse phases is reduced.In addition,the LiBr pre-modification layer at the buried interface minimizes the trap states and enhances the radiative recombination of perovskites.Accordingly,our PeLEDs show a champion external quantum efficiency(EQE)of 25.5%for 4 mm2 device,and 22.9%for 100 mm^(2)device.
基金support from the National Key R&D Program of China(Grant No.2023YFE0111500)the National Natural Science Foundation of China(Grant No.52321006,T2394480,T2394484,22109143,22479131)+8 种基金Beijing National Laboratory for Molecular Sciences(BNLMS-CXXM-202005)the China Postdoctoral Innovative Talent Support Program(Grant No.BX2021271)the China Postdoctoral Science Foundation(2022M712851)the Opening Project of State Key Laboratory of Advanced Technology for Float Glass(Grant No.2022KF04)Graduate Education Reform Project of Henan Province(Grant No.2023SJGLX136Y)Key R&D Special Program of Henan Province(Grant No.241111242000)Program for Science and Technology Innovation Talents in Universities of Henan Province(Grant No.25HASTIT005)Training Plan for Young Backbone Teachers of Zhengzhou University(Grant No.2023ZDGGJS017)the Joint Research Project of Puyang Shengtong Juyuan New Materials Co.,Ltd.(Grant No.20230128A).
文摘Organic-inorganic hybrid perovskite solar cells achieve remarkable efficiencies(>26%)yet face stability challenges.Quasi-2D alternating-cation-interlayer perovskites offer enhanced stability through hydrophobic spacer cations but suffer from vertical phase segregation and buried interface defects.Herein,we introduce dicyanodiamide(DCD)to simultaneously address these dual limitations in GA(MA)_(n)Pb_(n)I_(3n+1)perovskites.The guanidine group in DCD passivates undercoordinated Pb^(2+)and MA^(+)vacancies at the perovskite/TiO_(2)interface,while cyano groups eliminate oxygen vacancies in TiO_(2)via Ti^(4+)-CN coordination,reducing interfacial trap density by 73%with respect to the control sample.In addition,DCD regulates crystallization kinetics,suppressing low-n-phase aggregation and promoting vertical alignment of high-n phases,which benefit for carrier transport.This dual-functional modification enhances charge transport and stabilizes energy-level alignment.The optimized devices achieve a record power conversion efficiency of 21.54%(vs.19.05%control)and retain 94%initial efficiency after 1200 h,outperforming unmodified counterparts(84%retention).Combining defect passivation with phase homogenization,this work establishes a molecular bridge strategy to decouple stability-efficiency trade-offs in low-dimensional perovskites,providing a universal framework for interface engineering in high-performance optoelectronics.
