Enhancing the Performance of Perovskite Light-Emitting Diodes via Synergistic Effect of Defect Passivation and Dielectric Screening

Metal halide perovskites,particularly the quasi-two-dimensional perovskite subclass,have exhibited considerable potential for next-generation electroluminescent materials for lighting and display.Nevertheless,the presence of defects within these perovskites has a substantial influence on the emission efficiency and durability of the devices.In this study,we revealed a synergistic passivation mechanism on perovskite films by using a dual-functional compound of potassium bromide.The dual functional potassium bromide on the one hand can passivate the defects of halide vacancies with bromine anions and,on the other hand,can screen the charged defects at the grain boundaries with potassium cations.This approach effectively reduces the probability of carriers quenching resulting from charged defects capture and consequently enhances the radiative recombination efficiency of perovskite thin films,leading to a significant enhancement of photoluminescence quantum yield to near-unity values(95%).Meanwhile,the potassium bromide treatment promoted the growth of homogeneous and smooth film,facilitating the charge carrier injection in the devices.Consequently,the perovskite light-emitting diodes based on this strategy achieve a maximum external quantum efficiency of~21%and maximum luminance of~60,000 cd m^(-2).This work provides a deeper insight into the passivation mechanism of ionic compound additives in perovskite with the solution method.

Constructing Al@C-Sn pellet anode without passivation layer for lithium-ion battery

Al is considered as a promising lithium-ion battery(LIBs)anode materials owing to its high theoretical capacity and appropri-ate lithation/de-lithation potential.Unfortunately,its inevitable volume expansion causes the electrode structure instability,leading to poor cyclic stability.What’s worse,the natural Al2O3 layer on commercial Al pellets is always existed as a robust insulating barrier for elec-trons,which brings the voltage dip and results in low reversible capacity.Herein,this work synthesized core-shell Al@C-Sn pellets for LIBs by a plus-minus strategy.In this proposal,the natural Al2O3 passivation layer is eliminated when annealing the pre-introduced SnCl2,meanwhile,polydopamine-derived carbon is introduced as dual functional shell to liberate the fresh Al core from re-oxidization and alle-viate the volume swellings.Benefiting from the addition of C-Sn shell and the elimination of the Al2O3 passivation layer,the as-prepared Al@C-Sn pellet electrode exhibits little voltage dip and delivers a reversible capacity of 1018.7 mAh·g^(-1) at 0.1 A·g^(-1) and 295.0 mAh·g^(-1) at 2.0 A·g^(-1)(after 1000 cycles),respectively.Moreover,its diffusion-controlled capacity is muchly improved compared to those of its counterparts,confirming the well-designed nanostructure contributes to the rapid Li-ion diffusion and further enhances the lithium storage activity.

In-situ interfacial passivation and self-adaptability synergistically stabilizing all-solid-state lithium metal batteries

The function of solid electrolytes and the composition of solid electrolyte interphase(SEI)are highly significant for inhibiting the growth of Li dendrites.Herein,we report an in-situ interfacial passivation combined with self-adaptability strategy to reinforce Li_(0.33)La_(0.557)TiO_(3)(LLTO)-based solid-state batteries.Specifically,a functional SEI enriched with LiF/Li_(3)PO_(4) is formed by in-situ electrochemical conversion,which is greatly beneficial to improving interface compatibility and enhancing ion transport.While the polarized dielectric BaTiO_(3)-polyamic acid(BTO-PAA,BP)film greatly improves the Li-ion transport kinetics and homogenizes the Li deposition.As expected,the resulting electrolyte offers considerable ionic conductivity at room temperature(4.3 x 10~(-4)S cm^(-1))and appreciable electrochemical decomposition voltage(5.23 V)after electrochemical passivation.For Li-LiFePO_(4) batteries,it shows a high specific capacity of 153 mA h g^(-1)at 0.2C after 100 cycles and a long-term durability of 115 mA h g^(-1)at 1.0 C after 800 cycles.Additionally,a stable Li plating/stripping can be achieved for more than 900 h at 0.5 mA cm^(-2).The stabilization mechanisms are elucidated by ex-situ XRD,ex-situ XPS,and ex-situ FTIR techniques,and the corresponding results reveal that the interfacial passivation combined with polarization effect is an effective strategy for improving the electrochemical performance.The present study provides a deeper insight into the dynamic adjustment of electrode-electrolyte interfacial for solid-state lithium batteries.

Cross-layer all-interface defect passivation with pre-buried additive toward efficient all-inorganic perovskite solar cells

The buried interface in the perovskite solar cell(PSC)has been regarded as a breakthrough to boost the power conversion efficiency and stability.However,a comprehensive manipulation of the buried interface in terms of the transport layer,buried interlayer,and perovskite layer has been largely overlooked.Herein,we propose the use of a volatile heterocyclic compound called 2-thiopheneacetic acid(TPA)as a pre-buried additive in the buried interface to achieve cross-layer all-interface defect passivation through an in situ bottom-up infiltration diffusion strategy.TPA not only suppresses the serious interfacial nonradiative recombination losses by precisely healing the interfacial and underlying defects but also effectively enhances the quality of perovskite film and releases the residual strain of perovskite film.Owing to this versatility,TPA-tailored CsPbBr3 PSCs deliver a record efficiency of 11.23% with enhanced long-term stability.This breakthrough in manipulating the buried interface using TPA opens new avenues for further improving the performance and reliability of PSC.

Synergistic defect passivation and strain compensation toward efficient and stable perovskite solar cells

Rational interface engineering is essential for minimizing interfacial nonradiative recombination losses and enhancing device performance.Herein,we report the use of bidentate diphenoxybenzene(DPOB)isomers as surface modifiers for perovskite films.The DPOB molecules,which contain two oxygen(O)atoms,chemically bond with undercoordinated Pb^(2+) on the surface of perovskite films,resulting in compression of the perovskite lattice.This chemical interaction,along with physical regulations,leads to the formation of high-quality perovskite films with compressive strain and fewer defects.This compressive strain-induced band bending promotes hole extraction and transport,while inhibiting charge recombination at the interfaces.Furthermore,the addition of DPOB will reduce the zero-dimensional(OD) Cs_4PbBr_6 phase and produce the two-dimensional(2D) CsPb_(2)Br_5 phase,which is also conducive to the improvement of device performance.Ultimately,the resulting perovskite films,which are strain-released and defect-passivated,exhibit exceptional device efficiency,reaching 10.87% for carbon-based CsPbBr_(3) device,14.86% for carbon-based CsPbI_(2)Br device,22,02% for FA_(0.97)Cs_(0.03)PbI_(3) device,respectively.Moreover,the unencapsulated CsPbBr_(3) PSC exhibits excellent stability under persistent exposure to humidity(80%) and heat(80℃) for over 50 days.

Bifunctional passivation by lewis-base molecules for efficient printable mesoscopic perovskite solar cells

Printable mesoscopic perovskite solar cells(PM-PSCs)possess notable merits in terms of cost-effectiveness,easy manufacturing,and large scale applications.Nevertheless,the absence of a hole transport layer contributes to the exacerbation of carrier recombination,and the defects between the perovskite and electron transport layer(ETL)interfaces significantly decrease the efficiency of the devices.In this study,a bifunctional surface passivation approach is proposed by applying a thioacetamide(TAA)surfactant on the mesoporous TiO_(2)interface.The results demonstrate that TAA molecules could interact with TiO_(2),thereby diminishing the oxygen vacancy defects.Additionally,the amino group and sulfur atoms in TAA molecules act as Lewis base to effectively passivate the uncoordinated Pb^(2+)in perovskite and improve the morphology of perovskite,and decrease the trap-state density of perovskite.The TAA passivation mechanism improves the alignment of energy levels between TiO_(2)and perovskite,facilitating electron transport and reducing carrier recombination.Consequently,the TAA-passivated device achieved a champion power conversion efficiency(PCE)of 17.86%with a high fill factor(FF)of 79.16%and an open-circuit voltage(V_(OC))of 0.971 V.This investigation presents a feasible strategy for interfacial passivation of the ETL to further improve the efficiency of PM-PSCs.

Role of self-assembled molecules’anchoring groups for surface defect passivation and dipole modulation in inverted perovskite solar cells

Inverted perovskite solar cells have gained prominence in industrial advancement due to their easy fabrication,low hysteresis effects,and high stability.Despite these advantages,their efficiency is currently limited by excessive defects and poor carrier transport at the perovskite-electrode interface,particularly at the buried interface between the perovskite and transparent conductive oxide(TCO).Recent efforts in the perovskite community have focused on designing novel self-assembled molecules(SAMs)to improve the quality of the buried interface.However,a notable gap remains in understanding the regulation of atomic-scale interfacial properties of SAMs between the perovskite and TCO interfaces.This understanding is crucial,particularly in terms of identifying chemically active anchoring groups.In this study,we used the star SAM([2-(9H-carbazol-9-yl)ethyl]phosphonic acid)as the base structure to investigate the defect passivation effects of eight common anchoring groups at the perovskite-TCO interface.Our findings indicate that the phosphonic and boric acid groups exhibit notable advantages.These groups fulfill three key criteria:they provide the greatest potential for defect passivation,exhibit stable adsorption with defects,and exert significant regulatory effects on interface dipoles.Ionized anchoring groups exhibit enhanced passivation capabilities for defect energy levels due to their superior Lewis base properties,which effectively neutralize local charges near defects.Among various defect types,iodine vacancies are the easiest to passivate,whereas iodine-substituted lead defects are the most challenging to passivate.Our study provides comprehensive theoretical insights and inspiration for the design of anchoring groups in SAMs,contributing to the ongoing development of more efficient inverted perovskite solar cells.

Improved efficiency and stability of inverse perovskite solar cells via passivation cleaning

Amidst the global energy and environmental crisis,the quest for efficient solar energy utilization intensifies.Perovskite solar cells,with efficiencies over 26%and cost-effective production,are at the forefront of research.Yet,their stability remains a barrier to industrial application.This study introduces innovative strategies to enhance the stability of inverted perovskite solar cells.By bulk and surface passivation,defect density is reduced,followed by a"passivation cleaning"using Apacl amino acid salt and isopropyl alcohol to refine film surface quality.Employing X-ray diffraction(XRD),scanning electron microscope(SEM),and atomic force microscopy(AFM),we confirmed that this process effectively neutralizes surface defects and curbs non-radiative recombination,achieving 22.6%efficiency for perovskite solar cells with the composition Cs_(0.15)FA_(0.85)PbI_(3).Crucially,the stability of treated cells in long-term tests has been markedly enhanced,laying groundwork for industrial viability.

Doping PCBM with fullerene phosphinate derivatives enhances the interface energy alignment and synergistic passivation capability

Phenyl-C_(61)-butyric acid methyl ester(PCBM) serves as a common electron transport layer(ETL) in inverted p-i-n structure perovskite solar cells(IPSCs),yet energy barriers and insufficient passivation at the PCBM-perovskite interface hinder device effectiveness and durability.In this study,we present a series of novel Fullerene Phenylacid Ester Derivatives(FPEDs:FPP,FTPP,FDPP) incorporated into PCBM.Our investigations illustrate that FPEDs effectively act to passivate the perovskite surface by forming robust interactions with uncoordinated Pb^(2+) ions via the phosphine oxide groups present in their molecular structures,thereby enhancing the stability of the devices.Moreover,these additives elevate the energy level of the lowest unoccupied molecular orbital(LUMO) of ETL,diminish the electron injection barrier,and enhance the efficiency of interlayer electron transport.Incorporating FPEDs enhances ETL coverage on the perovskite layer,reducing leakage current significantly.Notably,Devices with PCBM/FTPP achieved a peak PCE of 23.62% and showed superior stability,maintaining 96,8% of the initial PCE after 500 h,while control devices retained merely 80.7% over the same period.

Zn Dissolution-Passivation Behavior with ZnO Formation via In Situ Characterizations

In this study,ZnO formation during the dissolution-passivation process of Zn anodes is observed via in situ Raman and optical characterization.The Zn passivation during galvanostatic anodization merely follows the dissolution-precipitation model,whereas that of potentiodynamic polarization exhibits different behaviors in different potential ranges.Initially,the Zn electrode is gradually covered by a ZnO precipitation film and then undergoes solid-state oxidation at~255 mV.The starting point of solid-state oxidation is well indicated by the abrupt current drop and yellow coloration of the electrode surface.During the pseudo passivation,an intense current oscillation is observed.Further,blink-like color changes between yellow and dark blue are revealed for the first time,implying that the oscillation is caused by the dynamic adsorption and desorption of OH groups.The as-formed ZnOs then experience a dissolution-reformation evolution,during which the crystallinity of the primary ZnO film is improved but the solid-state-formed ZnO layer becomes rich in oxygen vacancies.Eventually,oxide densification is realized,contributing to the Zn passivation.This study provides new insights into the Zn dissolution-passivation behavior,which is critical for the future optimization of Zn batteries.

Control method of chalcopyrite passivation in bioleaching

Passivation is a common phenomenon on the surface of chalcopyrite in the process of bioleaching. The ordinary leaching and strengthening leaching by adding glass beads were carried out. The results show that the passivation of chalcopyrite was greatly weakened in strengthening leaching due to the change of leaching conditions. The copper leaching efficiency was increased from 50% to 89.8% through adding beads. The SEM and X-ray diffraction （XRD） analyses illustrate that there are few jarosite precipitates and weak passivation on the surface of chalcopyrite in strengthening leaching. In contrast, there are thick and compact jarosite precipitate and obvious passivation in ordinary leaching, which hinders further dissolution of chalcopyrite.

Effect of impurities in recycling water on Pb-Ag anode passivation in zinc electrowinning process

Effect of impurities in recycling water on Pb-Ag anode passivation in zinc electrowinning process was investigated by linear scan voltammetry.Results show that passivation process would be affected in the presence of Cl^-and F-in recycling water.It was highly advantageous to take H2SO4 concentration as 180g/L,Mn^2＋ concentration as 3-5 g/L and F-less than 42mg/L.However,passivation process would not be affected when Cl^-concentration was less than 13mg/L without any other ions,or when mass ratio of Mn^2＋ to Cl^-existing in electrolyte was 8,where Cl^-concentration could reach up to 625mg/L.

High efficiency CZTSSe solar cells enabled by dual Ag-passivation approach via aqueous solution process

Ag substitution in Cu_(2)ZnSn(S,Se)_(4)(CZTSSe)is a promising way to mitigate Cu/Zn related defects,electrostatic fluctuations and Shockley-Read-Hall(SRH)recombination centers.However,high performance ACZTSSe solar cells are generally demonstrated with more Ag amounts and strenuous fabrication processes,which are not ideal when using cheap constituent materials CZTSSe.To reduce the Ag amount(2%-3%),local Ag substitutions into CZTSSe at front(F),back(B)and dual front/back(FB)were proposed.Experimental results revealed that F-passivation effectively reduced the Cu/Zn related defects and further limits the interface/bulk recombination whereas B-passivation improved the grain growth at the back interface and further allows enhanced transport of charge carriers.By employing the dual Agpassivation approach,the final ACZTSSe device parameters were significantly improved and remarkable power conversion efficiency(PCE)of 12.43%was achieved with eco-friendly aqueous solution process.

Evaporated potassium chloride for double-sided interfacial passivation in inverted planar perovskite solar cells

Defect-induced charge carrier recombination at the interfaces between perovskite and adjacent charge transport layers restricts further improvements in the device performance of perovskite solar cells(PSCs).Defect passivation at these interfaces can reduce trap states and inhibit the induced nonradiative recombination.Herein,we report a double-sided interfacial passivation via simply evaporating potassium chloride(DIP-KCl)at both the hole transport layer(HTL)/perovskite and perovskite/electron transport layer(ETL)interfaces in inverted planar PSCs.We demonstrate that the bottom KCl layer at the HTL/perovskite interface not only reduces the interfacial defects and improves the interfacial contact,but also leads to increased perovskite crystallinity,while the top KCl layer at the perovskite/ETL interface efficiently passivates the perovskite top surface defects and facilitates electron extraction at this interface.Thus,suppressed nonradiative recombination and faster charge extraction at both interfaces close to the perovskite layer can be achieved by using our DIP-KCl strategy.As a result,inverted PSCs based on DIP-KCl present an increased efficiency from 17.1% to 19.2% and enhanced stability,retaining over 90% of their initial efficiency after aging at maximum power point tracking for 1000 h.This work provides a simple and efficient way for defect passivation to further increase the efficiency and stability of PSCs.

考虑passivation的备件库存时变凸优化

考虑到passivation现象,利用时变库存平衡方程构建时变备件短缺数函数,根据扩展帕姆定理将当前时刻之前时段的累积需求率糅合入泊松分布的形状参数,建立考虑备件累积需求率的凸优化算法。以费用约束下的时变可用度为目标函数,利用凸优化算法,得到每一时段的最优配置方案。利用众数法,选择适当的全局库存策略。最后,构建了优化案例来阐释本文提出的方法,同时通过对比几种库存策略,证明了所提方法的优越性。

Cerium-tannic acid passivation treatment on galvanized steel

A novel cerium-tannic acid passivation treatment was performed on galvanized steel. The corrosion resistance of cerium-tannic passivated samples was tested by dropping test with 0.5 wt.% CuSO4 aqueous solution. The mass loss per unit area of passivated samples was measured after the corrosion in 0.5 mol/L NaCl ＋ 0.005 mol/L H2SO4 at room temperature for 96 h. The electrochemical behaviors of cerium, tannic acid, and cerium-tannic acid passivated samples on galvanized steel in 0.5 mol/L NaCl solution were investigated by polarization curves and electrochemical impendence spectra. The corrosion equivalent circuit was established according to the impedance characteristics. The results show that cerium-tannic acid treated samples exhibit better corrosion resistance than the sole cerium or tannic acid treated samples under the same condition. The mechanism of synergistic effect for cerium-tannic acid passivation on galvanized steel was discussed.

Passivation process of X80 pipeline steel in bicarbonate solutions

The passivation process of X80 pipeline steel in bicarbonate solutions was investigated using potentiodynamic, dynamic electro-chemical impedance spectroscopy （DEIS）, and Mott-Schottky measurements. The results show that the shape of polarization curves changes with concentration. The critical ＇passive＇ concentration is 0.009 mol/L for X80 pipeline steel in bicarbonate solutions. No anodic current peak exists in solutions when the concentration is lower than 0.009 mol/L, whereas there are one and two anodic current peaks when the concentration ranges from 0.009 to 0.05 mol/L and is higher than 0.1 mol/L, respectively. DEIS measurements show that there exist active dissolution range, transition range, pre-passive range, passive layer formation range, passive range, and trans-passive range for X80 pipeline steel in the 0.1 mol/L solutions. The results of DEIS measurements are in complete agreement with the potentiodynamic diagram. An equivalent circuit containing three sub-layers is used to explain the Nyquist plots in the passive range. Analyses are well made for explaining the corresponding fitted capacitance and impedance. The Mott-Schottky plots show that the passive film of X80 pipeline steel is an n-type semiconductor, and capacitance measurements are in good accordance with the results of DEIS experiment.

Relatedness between catalytic effect of activated carbon and passivation phenomenon during chalcopyrite bioleaching by mixed thermophilic Archaea culture at 65°C

The relatedness between catalytic effect of activated carbon and passivation phenomenon during chalcopyrite bioleachingby mixed thermophilic Archaea culture(Acidianus brierleyi,Metallosphaera sedula,Acidianus manzaensis and Sulfolobusmetallicus)at65°C was studied.Leaching experiments showed that the addition of activated carbon could significantly promote thedissolution of chalcopyrite for both bioleaching and chemical leaching.The results of synchrotron-based X-ray diffraction,ironL-edge and sulfur K-edge X-ray absorption near edge structure spectroscopy indicated that activated carbon could change thetransition path of electrons through galvanic interactions to form more readily dissolved secondary mineral chalcocite at a low redoxpotential(?400mV)and then enhanced the copper dissolution.Jarosite accumulated immediately in the initial stage of bioleachingwith activated carbon but copper dissolution was not hindered.However,much jarosite precipitated on the surface of chalcopyrite inthe late stage of bioleaching,which might account for the decrease of copper dissolution rate.More elemental sulfur(S0)was alsodetected with additional activated carbon but the mixed thermophilic Archaea culture had a great sulfur oxidation activity,thus S0waseliminated and seemed to have no significant influence on the dissolution of chalcopyrite.

Comparative study on the passivation layers of copper sulphide minerals during bioleaching

The bioleaching of copper sulphide minerals was investigated by using A. ferrooxidans ATF6. The result shows the preferential order of the minerals bioleaching as djurleite〉bomite〉pyritic chalcopyrite〉covellite〉porphyry chalcopyfite. The residues were characterized by X-ray diffraction （XRD） and scanning electron microscopy （SEM）. It is indicated that jarosite may not be responsible for hindered disso- lution. The elemental sulfur layer on the surface of pyritic chalcopyrite residues is cracked. The compact surface layer of porphyry chalcopy- rite may strongly hinder copper extraction. X-ray photoelectron spectroscopy （XPS） further confirms that the passivation layers of covellite, pyritic chalcopyrite, and porphyry chalcopyrite are copper-depleted sulphide Cu4S11, S8, and copper-rich iron-deficient polysulphide CtuFe2S9, resoectivelv. The ability of these oassivation layers was found as Cu4Fe2S9〉Cu4S11〉S8〉iarosite.

Perfection of Perovskite Grain Boundary Passivation by Rhodium Incorporation for Efficient and Stable Solar Cells

Organic cation and halide anion defects are omnipresent in the perovskite films,which will destroy perovskite electronic structure and downgrade the properties of devices.Defect passivation in halide perovskites is crucial to the application of solar cells.Herein,tiny amounts of trivalent rhodium ion incorporation can help the nucleation of perovskite grain and passivate the defects in the grain boundaries,which can improve efficiency and stability of perovskite solar cells.Through first-principle calculations,rhodium ion incorporation into the perovskite structure can induce ordered arrangement and tune bandgap.In experiment,rhodium ion incorporation with perovskite can contribute to preparing larger crystalline and uniform film,reducing trap-state density and enlarging charge carrier lifetime.After optimizing the content of 1% rhodium,the devices achieved an efficiency up to 20.71% without obvious hysteresis,from 19.09% of that pristine perovskite.In addition,the unencapsulated solar cells maintain 92% of its initial efficiency after 500 h in dry air.This work highlights the advantages of trivalent rhodium ion incorporation in the characteristics of perovskite solar cells,which will promote the future industrial application.