Lewis Acid-base Adducts Research Articles

Tailored Supramolecular Additives to Control the Crystallization Process and Morphology of MAPbI3.

Perovskite films feature unique optoelectronic properties, rendering them promising for electronic devices. The properties depend on the morphology on a broad range of length scales from nanometers to millimeters, influenced by a variety of factors. However, controlling the morphology is challenging. A tailored supramolecular additive, N, N'-bis(2-aminoethyl) terephthalamide is developed to control the intermediate and perovskite crystallization of methyl ammonium lead iodide (MAPbI3) and enhance the thermal and moisture stability in the final film. Reversible coordinative interactions of the carbonyl groups with Pb2+ ions via Lewis acid-base adduct and subsequent ion-ion interactions of the peripheral ammonium groups with the perovskite grain boundaries are combined which is stabilized by a strong hydrogen bonding pattern formed between the amide moieties of the additive molecules. Adding low amounts of this additive to the precursor solution significantly decelerates the structure formation and systematically reduces the crystallite size. Slower growth of the intermediate phases and the incorporation of the additive to the grain boundary is observed with multiple time-resolved techniques. Evidence for the formation of single-molecule interlayers between the MAPbI3 crystals and the presence of directed supramolecular interaction between additive molecules is shown. Transferability of this approach to other perovskites is anticipated, paving the way to improved processing control and stability.

Tailoring pyridine bridged chalcogen-concave molecules for defects passivation enables efficient and stable perovskite solar cells

Suppressing deep-level defects at the perovskite bulk and surface is indispensable for reducing the non-radiative recombination losses and improving efficiency and stability of perovskite solar cells (PSCs). In this study, two Lewis bases based on chalcogen-thiophene (n-Bu4S) and selenophene (n-Bu4Se) having tetra-pyridine as bridge are developed to passivate defects in perovskite film. The uncoordinated Pb2+ and iodine vacancy defects can interact with chalcogen-concave group and pyridine group through the formation of the Lewis acid-base adduct, particularly both the defects can be surrounded by concave molecules, resulting in effective suppression charge recombination. This approach enables a power conversion efficiency (PCE) as high as 25.37% (25.18% certified) for n-i-p PSCs with stable operation at 65 °C and 1-sun illumination for 1300 hours in N2 (ISOS-L-2 protocol), retaining 94% of the initial efficiency. Our work provides insight into the bowl-shaped Lewis base in defects passivation by coordinated strategy for high-performance photovoltaic devices.

Beyond Hydrolysis: Scalable, On-Demand Dihydrogen Release from NaBH4 enables Circular and Sustainable Process Design

Hydrogen storage in its elemental form poses significant safety and economic challenges. Metal hydrides, particularly sodium borohydride, offer a promising alternative because of their superior safety profiles and enhanced transportability. This study presents a scalable hydrogen release system based on sodium borohydride and commercially available alcohols and acids. The system enables rapid, controlled hydrogen generation achieving quantitative yields. Quantum chemical calculations were performed to propose a mechanism for the alcoholysis of NaBH4 with isopropyl alcohol (IPA) and acid present. It was demonstrated that the reaction proceeds via isopropoxy substituted borane derivatives BH(3-n)OiPrn (for n = 0, 1, 2, 3), which can form Lewis acid-base adducts with IPA. These Lewis acid-base adducts serve as reaction complexes for -bond metathesis, upon which an equivalent of hydrogen gas is released. Notably, the spent fuel can be regenerated to sodium borohydride using established chemical reactions, ensuring the system's sustainability and applicability for larger-scale hydrogen production

Improved Charge‐Transfer Doping in Crystalline Polymer for Efficient and Stable Perovskite Solar Cells

AbstractPerovskite solar cells (PSCs) have significant potential for next‐generation photovoltaic technology applications. However, the instability of hole transport layers (HTLs) becomes the major obstacle to long‐term operational devices, which are affected by the intrinsic thermal instability and loose structure of hole transport materials, as well as the hygroscopicity and migration of dopants. Here, poly(3‐hexylthiophene‐2,5‐diyl) (P3HT) is used as a model crystalline polymer to thoroughly investigate effective p‐type doping strategies and the underlying mechanism. According to Hard–Soft‐Acid–Base theory, the soft base P3HT is more likely to form a stable Lewis acid–base adduct with the reactive soft acid radical, resulting in a strong charge‐transfer interaction, thereby enhancing conductivity and regulating the energy band of the HTL. Meanwhile, the radical cation salt can promote pre‐nucleation to optimize the crystallization orientation of P3HT. The resulting PSCs exhibited the efficiency of 25.16%, which is the highest efficiency reported so far based on doped P3HT. In addition, the resulting devices demonstrated excellent stability, maintaining 96.5%, 96%, and 91% of their initial efficiency after aging under continuous illumination for 2028 h, at 85 °C for 1080 h, and at maximum power point (MPP) tracking under continuous 1 Sun illumination at 85 °C for 528 h, respectively.

Synthesis of Lewis Acid–Base Adducts between Trialkyltriels and Heavy Bis(trimethylsilyl)pnictogenides

Synthesis of Lewis Acid–Base Adducts between Trialkyltriels and Heavy Bis(trimethylsilyl)pnictogenides

Functionalized sp2 Carbon-Conjugated Covalent Organic Frameworks for Interfacial Modulation of Inverted Perovskite Solar Cells.

Interfacial modulation utilizing functional materials is proven to be crucial for obtaining high photovoltaic performance in lead halide perovskite solar cells (PSCs). This study investigates, for the first time, the utilization of a pyrene-based sp2 carbon-conjugated covalent organic framework (sp2c-COF) as an interfacial layer in inverted PSCs. Functionalized with cyano (-CN) Lewis base groups, the sp2c-COF exhibits a dual effect, simultaneously passivating both the NiOx and the perovskite layers. Detailed characterization results highlight the role of sp2c-COF in reducing the Ni3+ defect density in NiOx films and forming Lewis acid-base adducts with undercoordinated Pb2+ on the perovskite surfaces, thereby inhibiting interfacial redox reactions and suppressing non-radiative recombination. Moreover, sp2c-COF leads to improved crystallinity of perovskite films. Benefiting from the synergistic effects, sp2c-COF-modified devices delivered a champion efficiency of 17.64%. These findings underscore the potential of sp2c-COF as a functional interface material for PSCs, offering enhanced efficiency and stability. The study contributes to advancing the understanding and application of covalent organic frameworks in photovoltaic technologies.

Neutral Adducts of Molybdenum Hexafluoride: Structure and Bonding in MoF6(NC5H5) and MoF6(NC5H5)2.

The first Lewis acid base adducts of MoF6 and an organic base have been synthesized, i. e., MoF6(NC5H5) and MoF6(NC5H5)2. These adducts are structurally characterized with X-ray crystallography, showing that both adducts adopt capped trigonal prismatic structures. The MoF6(NC5H5) and MoF6(NC5H5)2 adducts are fluxional on the NMR time scale at room temperature. Two different fluorine environments could be resolved by 19F NMR spectroscopy at -80 °C for the 1 : 2 adduct, MoF6(NC5H5)2, whereas MoF6(NC5H5) remains fluxional at that temperature. Density functional theory (DFT) calculations aide the assignment of the infrared and Raman spectra. Natural Bond Order and Molecular Electrostatic Potential analyses elucidate the structures and properties of the MoF6 pyridine adducts. Regions of significantly higher molecular electrostatic potential, i. e., σ-holes, in trigonal prismatic compared to octahedral MoF6 rationalize the capped trigonal prismatic geometry of the adducts. Whereas MoF6(NC5H5) is stable at room temperature under exclusion of moisture, MoF6(NC5H5)2 decomposes at 60 °C in pyridine solvent, and the solid slowly decomposes at room temperature after 24 h.

Uncovering Factors Controlling Reactivity of Metal-TEMPO Reaction Systems in the Solid State and Solution.

Nitroxides find application in various areas of chemistry, and a more in-depth understanding of factors controlling their reactivity with metal complexes is warranted to promote further developments. Here, we report on the effect of the metal centre Lewis acidity on both the distribution of the O- and N-centered spin density in 2,2,6,6-tetramethylpiperidine-N-oxyl (TEMPO) and turning TEMPO from the O- to N-radical mode scavenger in metal-TEMPO systems. We use Et(Cl)Zn/TEMPO model reaction system with tuneable reactivity in the solid state and solution. Among various products, a unique Lewis acid-base adduct of Cl2Zn with the N-ethylated TEMPO was isolated and structurally characterised, and the so-called solid-state 'slow chemistry' reaction led to a higher yield of the N-alkylated product. The revealed structure-activity/selectivity correlations are exceptional yet are entirely rationalised by the mechanistic underpinning supported by theoretical calculations of studied model systems. This work lays a foundation and mechanistic blueprint for future metal/nitroxide systems exploration.

Asymmetric catalysis by chiral FLPs: A computational mini-review.

Steric hindrance in Lewis acid (LA) and Lewis base (LB) obstruct the Lewis acid-base adduct formation, and the pair was termed as frustrated Lewis pair (FLP). In the past 16years, the field of enantioselective catalysis by chiral FLPs has been slowly growing. It was shown that chiral LAs are significant as they are involved in the hydrogen transfer (HT) step to the imine, resulting in enantioselectivity. After H2 activation, the borohydride can exist in a number of plausible conformations and their stability is governed by the presence of noncovalent interaction through C-H····π and π····π interactions. However, LBs are not ideal for asymmetric induction as they compete with the imine substrate as a counter LB. Further, the proton transfer from chiral LB to the imine does not induce any chirality as chirality develops in the HT step. However, intramolecular FLPs with chiral scaffold are very efficient as they possess an optimum distance between LA and LB, which facilitates the H2 activation but precludes the adduct formation of the small molecules substrate with the LA component. This mini-review summarizes computational investigation involving chiral LA and LB, and discusses intramolecular FLPs in the enantioselective catalysis.

3-Thiophenemalonic Acid Additive Enhanced Performance in Perovskite Solar Cells.

The development of ambient-air-processable organic-inorganic halide perovskite solar cells (OIHPSCs) is a challenge necessary for the transfer of laboratory-scale technology to large-scale and low-cost manufacturing of such devices. Different approaches like additives, antisolvents, composition engineering, and different deposition techniques have been employed to improve the morphology of the perovskite films. Additives that can form Lewis acid-base adducts are known to minimize extrinsic impacts that trigger defects in ambient air. In this work, we used the 3-thiophenemalonic acid (3-TMA) additive, which possesses thiol and carboxyl functional groups, to convert PbI2, PbCl2, and CH3NH3I to CH3NH3PbI3 completely. This strategy is effective in regulating the kinetics of crystallization and improving the crystallinity of the light-absorbing layer under high relative humidity (RH) conditions (30-50%). As a result, the 3-TMA additive increases the yield of the power conversion efficiency (PCE) from 14.9 to 16.5% and its stability under the maximum power point. Finally, we found that the results of this work are highly relevant and provide additional inputs to the ongoing research progress related to additive engineering as one of the efficient strategies to reduce parasitic recombination and enhance the stability of inverted OIHPSCs in ambient environment processing.

Minimizing defect states through multidentate coordination and morphology regulation for enhancing the performance of inverted perovskite solar cells.

The diversity of the defects present in perovskite materials negatively impacts both the power conversion efficiency (PCE) and the long-term stability of perovskite solar cells (PSCs). The chemical passivation of these defects has been addressed through a multifunctional molecule, 4-((trifluoromethyl)thio)benzoic acid, that contains the carbonyl (CO) group, which exhibits a strong passivation effect by interacting with both the organic cation (FA+) and uncoordinated Pb2+ ionic defects while the sulfur (S) heteroatom passivates Pb2+ defects at the grain boundary and on the surfaces of the perovskite layer. Additionally, the CF3 group protects the perovskite film from ambient degradation as well as stabilizing the perovskite framework by forming hydrogen and coordination bonds with the FA+ cation and Pb2+ ions, respectively. The interaction between CO and Pb2+ forms a Lewis acid-base adduct that regulates grain growth during crystallization, enhancing the perovskite film's surface morphology as confirmed by SEM, AFM, and PL mapping. This reduces trap-assisted recombination of charged carriers, thereby enhancing their lifetime and transport, as observed from TRPL, KPFM, and c-AFM analyses. As a result of the combined effect of the additive molecule, the optimized device showed a marked improvement in efficiency rising from 16.54% in the pristine device to 20.87% with a reduction in hysteresis. Moreover, the optimized device shows enhancement of stability by retaining ∼86% normalized PCE after 40 days of storage under ambient conditions at 25 ± 3 °C and a relative humidity of ∼45-55%.

Complexation and disproportionation of group 4 metal (alkoxy) halides with phosphine oxides.

Group 4 Lewis acids are well-known catalysts and precursors for (non-aqueous) sol-gel chemistry. Titanium, zirconium and hafnium halides, and alkoxy halides are precursors for the controlled synthesis of nanocrystals, often in the presence of Lewis base. Here, we investigate the interaction of Lewis bases with the tetrahalides (MX4, X = Cl, Br) and metal alkoxy halides (MXx(OR)4-x, x = 1-3, R = OiPr, OtBu). The tetrahalides yield the expected Lewis acid-base adducts MX4L2 (L = tetrahydrofuran or phosphine oxide). The mixed alkoxy halides react with Lewis bases in a more complex way. 31P NMR spectroscopy reveals that excess of phosphine oxide yields predominantly the complexation product, while a (sub)stoichiometric amount of phosphine oxide causes disproportionation of the MXx(OR)4-x species into MXx+1(OR)3-x and MXx-1(OR)5-x. The combination of complexation and disproportionation yields an atypical Job plot. In the case of zirconium isopropoxy chlorides, we fitted the concentration of all observed species and extracted thermodynamic descriptors from the Job plot. The complexation equilibrium constant decreases in the series: ZrCl3(OiPr) > ZrCl2(OiPr)2 ≫ ZrCl(OiPr)3, while the disproportionation equilibrium constant follows the opposite trend. Using calculations at the DFT level of theory, we show that disproportionation is driven by the more energetically favorable Lewis acid-base complex formed with the more acidic species. We also gain more insight into the isomerism of the complexes. The disproportionation reaction turns out to be a general phenomenon, for titanium, zirconium and hafnium, for chlorides and bromides, and for isopropoxides and tert-butoxides.

Heterobimetallic complexes of Mo–μ-O–M (M = Ca, Sr, Ba) with alkaline earth metals based on a flexible dentate (Me3tacn)MoO3 unit as a metalloligand

In this paper, we discussed the connection characteristics of the neutral weak donor metalloligand (Me3tacn)MoO3∙H2O (1) (Me3tacn = 1,4,7-trimethyl-1,4,7-triazaocynonane) and the formation of Lewis acid base adducts on the nitrates of alkaline-earth metals. Five heterobimetallic complexes {η1-(Me3tacn)MoO3}Ca(η2-NO3)2(H2O)3 (2), [{η1-(Me3tacn)MoO3}Ca(η2-NO3)2{η2,μ2-(Me3tacn)MoO3}]2 (3), {η1-(Me3tacn)MoO3}4Ca(η2-NO3)2∙12H2O (4), [{η2,μ2-(Me3tacn)MoO3}Sr(H2O)6]2Cl4∙2H2O (5), and {η2-(Me3tacn)MoO3}4Ba(η2-NO3)2∙8H2O (6) were synthesized and the crystal structures of the complexes were determined by X-ray crystallography. It is found that the (Me3tacn)MoO3 metalloligand was of good connectivity and rich coordination modes. Moreover, the complexes were characterized by infrared, fluorescence and UV-vis spectroscopies. The stability of complexes 2−6 at different temperatures was analyzed by thermogravimetry, and the antibacterial activity of the complexes was explored by disk diffusion method.

Antisolvent-Free Heterogenous Nucleation Enabled by Employing 4-Tert-Butyl Pyridine Additive and Two-Step Annealing for Efficient CsPbI2Br Perovskite Solar Cells.

All inorganic perovskite based on CsPbI2Br has attracted significant attention due to its relatively thermal stable structure compare to its hybrid counterparts. With a wide bandgap of 1.9eV and excellent light absorption capability, it has been extensively explored for applications in indoor photovoltaics and as a front absorber in tandem devices. However, the uncontrollable crystallization process during solvent evaporation and thermal annealing leads to both macroscopic defects like cracks and microscopic defects such as voids. In this study, a metastable adduct with lead (II) halides by incorporating 4-tert-butyl pyridine as a volatile Lewis base monodentate ligand in the precursor solution is formed. The strategic preferential decomposition of the adduct during the early-stage low-temperature annealing facilitated the desorption of lead (II) halides, inducing antisolvent-free heterogenous nucleation. This, in turn, promoted crystal growth during subsequent high-temperature annealing, resulting in dense films with low defect density. As a result, a maximum open-circuit voltage of 1.30V is achieved with the champion power conversion efficiency of 16.5% in CsPbI2Br-based perovskite solar cell. The work reveals a new mechanism of using Lewis acid-base adduct to obtain high quality perovskite films other than hindering crystallization in traditional way.

Lewis Acid-Base Adducts of α-Amino Acid-Derived Silaheterocycles and N-Methylimidazole

In chloroform solution, the reaction of bis(tert-butylamino)dimethylsilane ((tBuNH)2SiMe2) and an α-amino acid (α-amino isobutyric acid, H2Aib; D-phenylglycine, H2Phg; L-valine, H2Val) in the presence of N-methylimidazole (NMI) gave rise to the formation of the pentacoordinate silicon complexes (Aib)SiMe2-NMI, (Phg)SiMe2-NMI and (Val)SiMe2-NMI, respectively. Therein, the amino acid building block was a di-anionic bidentate chelator at the silicon atom. In solution, the complexes were involved in rapid coordination–dissociation equilibria between the pentacoordinate Si complex (e.g., (Aib)SiMe2-NMI) and its constituents NMI and a five-membered silaheterocycle (e.g., (Aib)SiMe2), as shown by 29Si NMR spectroscopy. The energetics of the Lewis acid-base adduct formation and the competing solvation of the NMI molecule by chloroform were assessed with the aid of computational methods. In CDCl3 solution, deuteration of the silaheterocycle NH group proceeded rapidly, with more than 50% conversion within two days. Upon cooling to −44 °C, the chloroform solvates of the adducts (Aib)SiMe2-NMI and (Phg)SiMe2-NMI crystallized from their parent solutions and allowed for their single-crystal X-ray diffraction analyses. In both cases, the Si atom was situated in a distorted trigonal bipyramidal coordination sphere with equatorial Si–C bonds and an equatorial Si–N bond (the one of the silaheterocycle). The axial positions were occupied by a carboxylate O atom of the silaheterocycle and the NMI ligand’s donor-N-atom.

A Combination of B- and N-Doped π-Systems Enabling Systematic Tuning of Electronic Structures and Properties.

Doping heteroatoms into polycyclic aromatic hydrocarbons (PAHs) may alter their structures and thereby physical properties. This study reports the construction of B/N-codoped PAHs via combining the B- and N-doped π-systems. Two π-extended B/N-codoped PAHs were synthesized through the Mallory photoreaction. Both feature a C48 BN2 π-skeleton, which is assembled by linearly fusing three substructures including B-doped and sp2 -hybridized N-doped π-moieties and one pyrene unit. In comparison to the pristine B-doped analog, their intramolecular charge transfer (ICT) states are distinctly modulated by the fused N-doped π-system and the further incorporated cyano group, leading to their tunable optical properties, as revealed by detailed theoretical and experimental analysis. Furthermore, these three molecules have sufficient Lewis acidity and can coordinate with Lewis base to form Lewis acid-base adducts, and notably, such intermolecular complexation can further dynamically modulate their ICT transitions and thereby photophysical properties, such as producing blue, green and red fluorescence.

Multinuclear Zinc-Magnesium Hydroxide Carboxylates: A Predesigned Model System for Copolymerization of CO2 with Epoxides.

Among numerous catalysts in the ring-opening copolymerization of epoxides with carbon dioxide (CO2), zinc dicarboxylate complexes are the most common type, and in the family of metal-based homogeneous catalysts, zinc and magnesium complexes have attracted widespread attention. We report on the synthesis and structural characterization of a zinc-magnesium benzoate framework templated by the central hydroxide anion with μ3-κ2:κ2:κ2 coordination mode, [ZnMg2(μ3-OH)(O2CPh)5]n (n = 1 or 2). The resulting heterometallic system forms stable Lewis acid-base adducts with tetrahydrofuran (THF) and cyclohexene oxide (CHO), which crystallize as the hexanuclear zinc-magnesium hydroxide carboxylate cluster [ZnMg2(μ3-OH)(O2CPh)5(L)2]2 (L = THF or CHO). Their X-ray crystal structure analysis revealed that the Zn center prefers 4-fold coordination and the Mg centers demonstrated the ability to accommodate higher coordination numbers, and as a result, the heterocyclic molecules are exclusively bonded to 6-fold Mg atoms. The heteronuclear carboxylate aggregates appeared active in the copolymerization reaction at elevated temperatures to produce an alternating poly(cyclohexene carbonate).

1,8-Dihydroxy Naphthalene-A New Building Block for the Self-Assembly with Boronic Acids and 4,4'-Bipyridine to Stable Host-Guest Complexes with Aromatic Hydrocarbons.

The new Lewis acid-base adducts of general formula X(nad)B←NC5H4-C5H4N→B(nad)X [nad = 1,8-O2C10H6, X = C6H5 (2c), 3,4,5-F3-C6H2 (2d)] were synthesized in high yields via reactions of 1,8-dihydroxy naphthalene [nadH2] and 4,4'-bipyridine with the aryl boronic acids C6H5B(OH)2 and 3,4,5-F3-C6H2B(OH)2, respectively, and structurally characterized by multi-nuclear NMR spectroscopy and SCXRD. Self-assembled H-shaped Lewis acid-base adduct 2d proved to be effective in forming thermally stable host-guest complexes, 2d × solvent, with aromatic hydrocarbon solvents such as benzene, toluene, mesitylene, aniline, and m-, p-, and o-xylene. Crystallographic analysis of these solvent adducts revealed host-guest interactions to primarily occur via π···π contacts between the 4,4'-bipyridyl linker and the aromatic solvents, resulting in the formation of 1:1 and 1:2 host-guest complexes. Thermogravimetric analysis of the isolated complexes 2d × solvent revealed their high thermal stability with peak temperatures associated with the loss of solvent ranging from 122 to 147 °C. 2d, when self-assembled in an equimolar mixture of m-, p-, and o-xylene (1:1:1), preferentially binds to o-xylene. Collectively, these results demonstrate the ability of 1,8-dihydroxy naphthalene to serve as an effective building block in the selective self-assembly to supramolecular aggregates through dative covalent N→B bonds.

Enhancing the Performance of Perovskite Solar Cells by Introducing 4-(Trifluoromethyl)-1H-imidazole Passivation Agents.

Defects in perovskite films are one of the main factors that affect the efficiency and stability of halide perovskite solar cells (PSCs). Uncoordinated ions (such as Pb2+, I-) act as trap states, causing the undesirable non-radiative recombination of photogenerated carriers. The formation of Lewis acid-base adducts in perovskite directly involves the crystallization process, which can effectively passivate defects. In this work, 4-(trifluoromethyl)-1H-imidazole (THI) was introduced into the perovskite precursor solution as a passivation agent. THI is a typical amphoteric compound that exhibits a strong Lewis base property due to its lone pair electrons. It coordinates with Lewis acid Pb2+, leading to the reduction in defect density and increase in crystallinity of perovskite films. Finally, the power conversion efficiency (PCE) of PSC increased from 16.49% to 18.97% due to the simultaneous enhancement of open-circuit voltage (VOC), short circuit current density (JSC) and fill factor (FF). After 30 days of storage, the PCE of the 0.16 THI PSC was maintained at 61.9% of its initial value, which was 44.3% for the control device. The working mechanism of THI was investigated. This work provides an attractive alternative method to passivate the defects in perovskite.

Precursor Solution Aging: A Universal Strategy Modulating Crystallization of Two-Dimensional Tin Halide Perovskite Films

Two-dimensional (2D) tin (Sn2+)-based perovskites have achieved remarkable advancements in (opto)electronic devices. However, fabricating high-quality and reproducible Sn halide perovskite thin films remains challenging due to uncontrollably fast crystallization. To overcome this issue, dimethyl sulfoxide has been incorporated as an indispensable strategy to form Lewis acid–base adducts but also has been proven to induce an irreversible Sn2+ oxidization effect. As the crystalline films grow directly from solution, a better understanding of precursor colloidal chemistry and the film formation process is critical. In this study, we report a universal solution aging approach to fabricate high-quality and reliable 2D Ruddlesden–Popper and Dion–Jacobson Sn2+ perovskite films and devices. The proper solution aging stabilizes the precursor colloids by eliminating aggregated complex and unreacted precursor clusters in the fresh precursor, leading to homogeneous nucleation/crystallization and film growth. The precursor aging reduced film defect density by nearly 2 orders of magnitude and improved charge transport mobility by over 5 times. This study can inspire the community to understand the deposition mechanism for high-quality Sn2+ perovskite thin films and promote the development of high-performance and reproducible Sn2+ perovskite based (opto)electronic devices.