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.

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.

Passivation engineering via silica‐encapsulated quantum dots for highly sensitive photodetection

Organometal halide perovskites are promising semiconducting materials for photodetectors because of their favorable optoelectrical properties.Although nanoscale perovskite materials such as quantum dots(QDs)show novel behavior,they have intrinsic stability issues.In this study,an effectively silane barrier-capped quantum dot(QD@APDEMS)is thinly applied onto a bulk perovskite photosensitive layer for use in photodetectors.QD@APDEMS is synthesized with a silane ligand with hydrophobic CH_(3)-terminal groups,resulting in excellent dispersibility and durability to enable effective coating.The introduction of the QD@APDEMS layer results in the formation of a lowdefect perovskite film with enlarged grains.This is attributed to the grain boundary interconnection effect via interaction between the functional groups of QD@APDEMS and uncoordinated Pb^(2+)in grain boundaries.By passivating the grain boundaries,where various trap sites are distributed,hole chargecarrier injection and shunt leakage can be suppressed.Also,from the energy point of view,the deep highest occupied molecular orbital(HOMO)level of QD@APDEMS can work as a hole charge injection barrier.Improved charge dynamics(generation,transfer,and recombination properties)and reduced trap density of QD@APDEMS are demonstrated.When this perovskite film is used in a photodetector,the device performance(especially the detectivity)stands out among existing perovskites evaluated for energy sensing device applications.

Mixed Cations Enabled Combined Bulk and Interfacial Passivation for Efficient and Stable Perovskite Solar Cells

Here,we report a mixed GAI and MAI(MGM)treatment method by forming a 2D alternating-cation-interlayer(ACI)phase(n=2)perovskite layer on the 3D perovskite,modulating the bulk and interfacial defects in the perovskite films simultaneously,leading to the suppressed nonradiative recombination,longer lifetime,higher mobility,and reduced trap density.Consequently,the devices’performance is enhanced to 24.5%and 18.7%for 0.12 and 64 cm^(2),respectively.In addition,the MGM treatment can be applied to a wide range of perovskite compositions,including MA-,FA-,MAFA-,and CsFAMA-based lead halide perovskites,making it a general method for preparing efficient perovskite solar cells.Without encapsulation,the treated devices show improved stabilities.

Phase Regulation and Defect Passivation Enabled by Phosphoryl Chloride Molecules for Efficient Quasi‑2D Perovskite Light‑Emitting Diodes

Quasi-2D perovskites have attracted tremendous interest for application as lightemission layers in light-emitting diodes(LEDs).However,the heterogeneous n phase and non-uniform distribution still severely limit the further development of quasi-2D perovskite LEDs(Pero-LEDs).Meanwhile,the increased defect density caused by the reduced dimension and grain size induces non-radiative recombination and further deteriorates the device performance.Here,we found that a series of molecules containing phosphoryl chloride functional groups have noticeable enhancement effects on the device performance of quasi-2D Pero-LEDs.Then,we studied the modification mechanism by focusing on the bis(2-oxo-3-oxazolidinyl)phosphinic chloride(BOPCl).It is concluded that the BOPCl can not only regulate the phase distribution by decreasing the crystallization rate but also remain in the grain boundaries and passivate the defects.As a result,the corresponding quasi-2D Pero-LEDs obtained a maximum external quantum efficiency(EQE_(max))of 20.82%and an average EQE(EQE_(ave))of around 20%on the optimal 50 devices,proving excellent reproducibility.Our work provides a new selection of molecular types for regulating the crystallization and passivating the defects of quasi-2D perovskite films.

Efficient Semi‑Transparent Wide‑Bandgap Perovskite Solar Cells Enabled by Pure‑Chloride 2D‑Perovskite Passivation

Wide-bandgap(WBG)perovskite solar cells suffer from severe non-radiative recombination and exhibit relatively large opencircuit voltage(V_(OC))deficits,limiting their photovoltaic performance.Here,we address these issues by in-situ forming a well-defined 2D perovskite(PMA)_(2)PbCl_(4)(phenmethylammonium is referred to as PMA)passivation layer on top of the WBG active layer.The 2D layer with highly pure dimensionality and halide components is realized by intentionally tailoring the side-chain substituent at the aryl ring of the post-treatment reagent.First-principle calculation and single-crystal X-ray diffraction results reveal that weak intermolecular interactions between bulky PMA cations and relatively low cation-halide hydrogen bonding strength are crucial in forming the well-defined 2D phase.The(PMA)_(2)PbCl_(4)forms improved type-I energy level alignment with the WBG perovskite,reducing the electron recombination at the perovskite/hole-transport-layer interface.Applying this strategy in fabricating semi-transparent WBG perovskite solar cells(indium tin oxide as the back electrode),the V_(OC)deficits can be reduced to 0.49 V,comparable with the reported state-of-the-art WBG perovskite solar cells using metal electrodes.Consequently,we obtain hysteresis-free 18.60%-efficient WBG perovskite solar cells with a high V_(OC)of 1.23 V.

Surface Passivation Toward Efficient and Stable Perovskite Solar Cells

Although metal halide perovskites are increasingly popular for the next generation of efficient photovoltaic devices,the inevitable defects from the preparation process have become the notorious barrier to further improvement of performance,which increases non-radiative recombination and lowers the power conversion efficiency of solar cells.Surface passivation strategies have been affirmed as one of the most practical approaches to suppress these defects.Therefore,it is necessary to have a detailed review on the surface passivation to reveal the improvements of the devices.Herein,the mechanism and recent advances of surface passivation have been systematically summarized with respect to various passivation approaches,including the Lewis acid–base,the low-dimensional perovskite,inorganic molecules,and polymers.Finally,the review also offers the research trend and prospects of surface passivation.

Sodium Nitrate Passivation as a Novel Insulation Technology for Soft Magnetic Composites

Sodium nitrate passivation has been developed as a new insulation technology for the production of FeSiAl soft magnetic composites (SMCs). In this work, the evolution of coating layers grown at different pH values is investigated involving analyses on their composition and microstructure. An insulation coating obtained using an acidic NaNO_(3) solution is found to contain Fe2O_(3), SiO_(2), Al2O_(3), and AlO(OH). The Fe2O_(3) transforms into Fe3O4 with weakened oxidizability of the NO_(3)– at an elevated pH, whereas an alkaline NaNO_(3) solution leads to the production of Al2O_(3), AlO(OH), and SiO_(2). Such growth is explained from both thermodynamic and kinetic perspectives and is correlated to the soft magnetic properties of the FeSiAl SMCs. Under tuned passivation conditions, optimal performance with an effective permeability of 97.2 and a core loss of 296.4 mW∙cm−3 is achieved at 50 kHz and 100 mT.

Boosting efficiency and stability of 2D alternating cation perovskite solar cells via rational surface-modification: Marked passivation efficacy of anion

Two-dimensional(2D) alternating cation(ACI) perovskite surface defects,especially dominant iodine vacancies(V_Ⅰ) and undercoordinated Pb^(2+),limit the performance of perovskite solar cells(PVSCs).To address the issue,1-butyl-3-methylimidazolium trifluoro-methane-sulfonate(BMIMOTF) and its iodide counterpart(BMIMI) are utilized to modify the perovskite surface respectively.We find that BMIMI can change the perovskite surface,whereas BMIMOTF shows a nondestructive and more effective defect passivation,giving significantly reduced defect density and suppressed charge-carrier nonradiative recombination.This mainly attributes to the marked passivation efficacy of OTF-anion on V_Ⅰ and undercoordinated Pb^(2+),rather than BMIMI^(+) cation.Benefiting from the rational surface-modification of BMMIMOTF,the films exhibit an optimized energy level alignment,enhanced hydrophobicity and suppressed ion migration.Consequently,the BMIMOTF-modified devices achieve an impressive efficiency of 21.38% with a record open-circuit voltage of 1.195 V,which is among the best efficiencies reported for 2D PVSCs,and display greatly enhanced humidity and thermal stability.

Unraveling abnormal buried interface anion defect passivation mechanisms depending on cation-induced steric hindrance for efficient and stable perovskite solar cells

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.

Back interface passivation for ultrathin Cu(In,Ga)Se_(2) solar cells with Schottky back contact: A trade-off of electrical effects

Back interface passivation reduces the back recombination of photogenerated electrons, whereas aggravates the blocking of hole transport towards back contact, which complicate the back interface engineering for ultrathin CIGSe solar cells with a Schottky back contact. In this work, theoretical explorations were conducted to study how the two contradictory electrical effects impact cell performance. For ultrathin CIGSe solar cells with a pronounced Schottky potential barrier(E_(h)> 0.2 eV), back interface passivation produces diverse performance evolution trends, which are highly dependent on cell structures and properties. Since a back Ga grading can screen the effect of reduced recombination of photogenerated electrons from back interface passivation, the hole blocking effect predominates and back interface passivation is not desirable. However, when the back Schottky diode merges with the main pn junction due to a reduced absorber thickness,the back potential barrier and the hole blocking effect is much reduced on this occasion. Consequently, cells exhibit the same efficiency evolution trend as ones with an Ohmic contact, where back interface passivation is always advantageous.The discoveries imply the complexity of back interface passivation and provide guidance to manipulate back interface for ultrathin CIGSe solar on TCOs with a pronounced Schottky back contact.

Recent Progress of Surface Passivation Molecules for Perovskite Solar Cell Applications

Due to the solution processable nature,the prepared perovskite films are polycrystalline with considerable number of defects.These defects,especially defects at interface accelerate the carrier recombination and reduce the carrier collection.Besides,the surface defects also affect the long-term stability of the perovskite solar cells(PVSCs).To solve this problem,surface passivation molecules are introduced at selective interface(the interface between perovskite and carrier selective layer).This review summarizes recent progress of small molecules used in PVSCs.Firstly,different types of defect states in perovskite films are introduced and their effects on device performance are discussed.Subsequently,surface passivation molecules are divided into four categories,and the interaction between the functional groups of the surface passivation molecules and selective defect states in perovskite films are highlighted.Finally,we look into the prospects and challenges in design noble small molecules for PVSCs applications.

In Situ Iodide Passivation Toward Efficient CsPbI_(3) Perovskite Quantum Dot Solar Cells

All-inorganic CsPbI_3 quantum dots(QDs) have demonstrated promising potential in photovoltaic(PV) applications. However, these colloidal perovskites are vulnerable to the deterioration of surface trap states, leading to a degradation in efficiency and stability. To address these issues, a facile yet effective strategy of introducing hydroiodic acid(HI) into the synthesis procedure is established to achieve high-quality QDs and devices. Through an in-depth experimental analysis, the introduction of HI was found to convert PbI_2 into highly coordinated [PbI_m]~(2-m), enabling control of the nucleation numbers and growth kinetics. Combined optical and structural investigations illustrate that such a synthesis technique is beneficial for achieving enhanced crystallinity and a reduced density of crystallographic defects. Finally, the effect of HI is further reflected on the PV performance. The optimal device demonstrated a significantly improved power conversion efficiency of 15.72% along with enhanced storage stability. This technique illuminates a novel and simple methodology to regulate the formed species during synthesis, shedding light on ofurther understanding solar cell performance, and aiding the design of future novel synthesis protocols for high-performance optoelectronic devices.

Anti-Corrosion and Reconstruction of Surface Crystal Plane for Zn Anodes by an Advanced Metal Passivation Technique

For the aqueous Zn-ion battery,dendrite formation,corrosion,and interfacial parasitic reactions are major issues,which greatly inhibits their practical application.How to develop a method of Zn construction or treatment to solve these issues for Zn anodes are still great challenges.Herein,a simple and cheap metal passivation technique is proposed for Zn anodes from a corrosion science perspective.Similar to the metal anticorrosion engineering,the formed interfacial protective layer in a chemical way can sufficiently solve the corrosion issues.Furthermore,the proposed passivity approach can reconstruct Zn surface-preferred crystal planes,exposing more(002)planes and improving surface hydrophilicity,which inhibits the formation of Zn dendrites and hydrogen evolution effectively.As expected,the passivated Zn achieves outstanding cycling life(1914 h)with low voltage polarization(<40 mV).Even at 6 mA cm^(−2) and 3 mA h cm^(−2),it can achieve stable Zn deposition over 460 h.The treated Zn anode coupled with MnO_(2) cathode shows prominently reinforced full batteries service life,making it a potential Zn anode candidate for excellent performance aqueous Zn-ion batteries.The proposed passivation approach provides a guideline for other metal electrodes preparation in various batteries and establishes the connections between corrosion science and batteries.

Passivation of PEA^(+)to CsPbI_(3)(110)Surface States:From the First Principles Calculations

This work investigates the effect of passivation on the electronic properties of inorganic perovskite CsPbI_(3)materials by using first-principles calculations with density functional theory(DFT).The passivation effect after the addition of Phenylethylamine(PEA+)molecule to CsPbI_(3)(110)surface is studied.The results of density of states(DOS)calculations show that the CsPbI_(3)(110)surface model with I atom terminated reveals new electronic DOS peaks(surface states)near the Fermi level.These surface states are mainly due to the contribution of I-5p orbital and are harmful to the CsPbI_(3)-based solar cells because they reduce the photoelectric conversion efficiency.The surface states near the Fermi level are significantly reduced,and the decline rate reaches 38.8%with the addition with PEA+molecule to the CsPbI3(110)surface.

Enhanced efficiency of the Sb_(2)Se_(3)thin-film solar cell by the anode passivation using an organic small molecular of TCTA

Antimony selenide(Sb_(2)Se_(3))is an emerging solar cell material.Here,we demonstrate that an organic small molecule of 4,4',4''-tris(carbazol-9-yl)-triphenylamine(TCTA)can efficiently passivate the anode interface of the Sb_(2)Se_(3)solar cell.We fabricated the device by the vacuum thermal evaporation,and took ITO/TCTA(3.0 nm)/Sb_(2)Se_(3)(50 nm)/C60(5.0 nm)/Alq3(3.0 nm)/Al as the device architecture,where Alq3 is the tris(8-hydroxyquinolinato)aluminum.By introducing a TCTA layer,the open-circuit voltage is raised from 0.36 to 0.42 V,and the power conversion efficiency is significantly improved from 3.2%to 4.3%.The TCTA layer not only inhibits the chemical reaction between the ITO and Sb_(2)Se_(3)during the annealing process but it also blocks the electron diffusion from Sb_(2)Se_(3)to ITO anode.The enhanced performance is mainly attributed to the suppression of the charge recombination at the anode interface.

Dramatic reduction in dark current ofβ-Ga_(2)O_(3) ultraviolet photodectors viaβ-(Al_(0.25)Ga_(0.75))_(2)O_(3) surface passivation

Solar-blind ultraviolet photodetectors with metal-semiconductor-metal structure were fabricated based onβ-(Al_(0.25)Ga_(0.75))_(2)O_(3)/β-Ga_(2)O_(3) film grown by metal-organic chemical vapor deposition.It was known that various surface states increase dark current and a large number of defects can hinder the transport of carriers,resulting in low switching ratio and low responsivity of the device.In this work,β-(Al_(0.25)Ga_(0.75))_(2)O_(3) films are used as surface passivation materials.Owning to its wide band gap,we obtain excellent light transmission and high lattice matching withβ-Ga_(2)O_(3).We explore the change and mechanism of the detection performance of theβ-Ga_(2)O_(3) detector afterβ-(Al_(0.25)Ga_(0.75))_(2)O_(3) surface passivation.It is found that under the illumination with 254 nm light at bias 5 V,theβ-(Al_(0.25)Ga_(0.75))_(2)O_(3)/β-Ga_(2)O_(3)photodetectors show dark current of just 18 pA and high current on/off ratio of 2.16×10^(5).The dark current is sharply reduced about 50 times after passivation of theβ-Ga_(2)O_(3) surface,and current on/off ratio increases by approximately 2 times.It is obvious thatβ-Ga_(2)O_(3) detectors withβ-(Al_(0.25)Ga_(0.75))_(2)O_(3) surface passivation can offer superior detector performance.

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。