Articles published on Boundary Defects
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- Research Article
- 10.1002/adma.73024
- May 1, 2026
- Advanced materials (Deerfield Beach, Fla.)
- Dongfang Xu + 11 more
All-inorganic CsPbI3 inverted perovskite solar cells (PSCs) suffer from severe nonradiative recombination and interfacial defects, which limit their efficiency and stability. To address this, we developed an interface engineering strategy based on CsPbBr3 quantum dots anchored in pore-size-tuned mesoporous silica nanoparticles (CPBQDs@MSNs), constructing a CsPbI3/CPBQDs@MSNs heterojunction. Notably, CPBQDs@M-MSNs (∼8nm) match the exciton Bohr radius of CsPbBr3 (∼7nm), enabling optimal exciton-photon critical coupling. This coupling strongly suppresses nonradiative recombination and thermal activation of defects, leading to superior fluorescence stability over a broad temperature range. The CPBQDs@MSNs treatment further enhances crystallinity, reduces grain boundary defects, and optimizes interfacial energy level alignment, thereby facilitating efficient charge-transport. Consequently, the inverted CsPbI3 PSCs achieve a remarkable power conversion efficiency (PCE) of 22.15%, the highest value for such devices, along with a record open-circuit voltage (VOC) of 1.28V. The devices exhibit excellent stability, retaining 93.16% of their initial PCE after 1300h in ambient air and 98.14% after 1000h of continuous illumination. This work highlights the crucial role of size-controlled QDs in interfacial engineering and offers a promising strategy for developing high-performance and stable perovskite optoelectronic devices.
- Research Article
- 10.1016/j.actamat.2026.122042
- May 1, 2026
- Acta Materialia
- Yujue Wang + 4 more
Strength-ductility synergy in diamond-nanoparticle-dispersed nanotwinned Cu with defective twin boundaries
- Research Article
- 10.1038/s41586-026-10415-9
- Apr 22, 2026
- Nature
- Yuwei Zhang + 14 more
All-solid-state batteries promise improved safety and higher energy density by replacing flammable liquid electrolytes and graphite anodes with solid electrolytes and lithium metal1-4. However, the penetration of soft lithium dendrites into hard ceramic electrolytes remains a substantial obstacle to realizing all-solid-state lithium metal batteries5-7. The mechanism by which mechanically soft lithium dendrites fracture hard ceramic electrolytes remains under debate7-10 owing to the challenges of characterizing nanoscale lithium distribution and its microstructure at the dendrite tip11. Here we investigate the fracture process driven by lithium dendrites in garnet electrolytes using multiscale cryogenic electron microscopy and micromechanical fracture models. We directly visualize lithium dendrites fully filling nanoscale crack tips and extending into micrometre-scale cracks. Limited crystal lattice rotation and plasticity in lithium dendrites indicate that the plated lithium generates substantial hydrostatic stress, which induces tensile stress in the solid electrolyte and drives both intergranular and transgranular fracture. By contrast, the region ahead of the lithium dendrite tip shows no measurable enrichment of lithium or lithium metal nuclei. The mechanically driven lithium penetration in garnet solid electrolyte can be redirected by geometrically engineered voids in the electrolyte, thus mitigating short-circuiting. Our findings suggest that grain boundary toughening and defect engineering are effective strategies for designing dendrite-resistant solid electrolytes.
- Research Article
- 10.1063/5.0317780
- Apr 13, 2026
- Journal of Applied Physics
- Zhenhua Chen + 5 more
Metal halide perovskites have recently begun to flourish in the field of optoelectronics. However, the inherent instability and grain boundary defects of traditional three-dimensional (3D) and two-dimensional (2D) polycrystalline films remain significant obstacles hindering their commercialization. Consequently, one-dimensional (1D) halide perovskite single crystals (PSCs) have garnered considerable attention due to their unique “molecular wire” structures. This distinctive structural constraint endows 1D PSCs with exceptional physical properties: strong quantum and dielectric confinement effects, broadband emission driven by self-trapped excitons, significant optoelectronic anisotropy, and excellent environmental stability. This article reviews the recent advances in 1D halide PSCs. We systematically explore the fundamental crystal structures and their derived photophysical properties, with a focus on elucidating the mechanisms behind their high quantum yields and nonlinear optical responses. Furthermore, various single-crystal growth strategies, ranging from slow cooling crystallization and inverse temperature crystallization to space-confined synthesis, are critically analyzed. Finally, we summarize the cutting-edge applications of 1D PSCs in high-performance UV–vis photodetectors, x-ray detectors, light-emitting diodes, and emerging polarization-sensitive devices.
- Research Article
- 10.1177/16878132261442325
- Apr 1, 2026
- Advances in Mechanical Engineering
- Zhen Liu + 3 more
The detection of metal surface defects is crucial in the field of industrial production. However, in practical applications, challenges such as ambiguous defect directions, large scale differences, and strong background interference are often encountered. This paper proposes an improved multi-scale fine-grained object detection framework based on YOLOv11, referred to as “DA-YOLO.” Firstly, the 3D attention module (3DAM) was used to enhance the model’s ability to model spatial direction features and improve the model’s ability to perceive fine-grained structures. Secondly, a feature enhancement module (AMFEM) employing multi-scale convolution and a spatial-channel attention mechanism was constructed, significantly boosting the model’s recognition accuracy for multi-scale targets and blurry boundary defects. Furthermore, an intersection and union ratio Aware Joint Loss function (IoU-Aware joint loss, IAJ-Loss) was proposed and designed, which further enhanced the quality perception ability and stability of the model in complex detection scenarios. The experimental results show that the DA-YOLO model improved mAP@0.5 by 5.42% and 4.05% respectively on the GC10-DET and NEU-DET datasets compared to the baseline YOLOv11 model, demonstrating superior defect detection performance.
- Research Article
- 10.1002/bkcs.70136
- Mar 18, 2026
- Bulletin of the Korean Chemical Society
- Lei Chen + 1 more
Abstract Mixed Sn–Pb perovskites provide the 1.2–1.3 eV narrow‐bandgap absorber needed for high efficiency of all perovskite tandems, but their deployment is limited by operational instability under light. This review synthesizes mechanistic origins and recent mitigation strategies for mixed Sn–Pb perovskite solar cells. The oxidation of Sn 2+ to Sn 4+ , often driven by iodine formation under light and bias, is the primary failure pathway; it creates Sn vacancies, self‐doping, and nonradiative loss. Surface/grain‐boundary defects, halide migration, reactive oxygen species, and interfacial redox at charge‐transport layers, along with hole accumulation from poor band alignment, further accelerate Sn–Pb perovskite degradation. Here we survey recent stability advances across additive chemistry, surface and grain‐boundary passivation, buried‐interface redesign with modified or alternative hole transport layers, and solvent systems that preserve Sn 2+ and correct Sn–Pb speciation for scalable coating. Together, these recent advances have enabled devices to retain 80%–90% output for hundreds to over a thousand hours. Lastly, we provide our perspectives on further improving the operational stability of Sn–Pb perovskite and solar cells.
- Research Article
- 10.1073/pnas.2524790123
- Mar 3, 2026
- Proceedings of the National Academy of Sciences
- Abdolvahab Seif + 8 more
Graphene supported on Si(111) (short Gr/Si) is one of the very few examples of a metal-free carbon catalyst that catalyzes gas-surface reactions. Kinetics measurements indicate dissociation of SO2 and H2S but molecular adsorption of N2O. In addition, spectroscopy revealed adsorbed sulfur after SO2 and H2S adsorption. Experiments were conducted at ultrahigh vacuum conditions, using kinetics techniques [i.e., thermal desorption spectroscopy (TDS)], spectroscopy [Auger electron spectroscopy (AES), Raman, X-ray photoelectron spectroscopy (XPS)], and imaging techniques [scanning tunneling microscopy (STM), low-energy electron diffraction]. Deviations of the gas-phase fragmentation pattern and multimass TDS pattern were observed. AES revealed adsorbed sulfur after SO2 and H2S adsorption. Thus, SO2 and H2S decompose, which contrasts with N2O, where only the molecular pathway was present. Density functional theory (DFT) confirms experimental observations. Whereas pristine Gr/Si is nonreactive, DFT modeled grain boundary defects (GBD) (as seen by STM) are the active sites for the decomposition. GBD consist of interfacial defects and surface defects (as seen by XPS). Because carbon and silicon are inexhaustible, Gr-based metal-free catalysts would be a paradigm change. Moreover, breaking H2S down into H2 would allow for recycling that waste gas and synthesizing green hydrogen.
- Research Article
- 10.26599/emd.2026.9370088
- Mar 1, 2026
- Energy Materials and Devices
- Zhuo Peng + 10 more
Perovskite solar cells (PSCs) have attracted considerable attention as next-generation photovoltaic technologies owing to their solution processability, low weight, and mechanical flexibility. Despite rapid progress, defect-induced nonradiative recombination remains a major obstacle, hindering further improvements in device efficiency and operational stability. In this work, we introduce 1H-indole-3-carbohydrazide (1H-CBH) as a multifunctional molecular additive that effectively mitigates these issues through synergistic defect passivation. Specifically, 1H-CBH simultaneously coordinates with undercoordinated Pb<sup>2+</sup> ions and forms hydrogen bonds with uncoordinated I<sup>-</sup> ions and formamidinium (FA<sup>+</sup>) cations. This dual interaction strategy promotes larger grain growth, reduces grain boundary defect density, and enhances interfacial compatibility with the electron-transport layer (ETL), thereby enabling improved charge transport. As a result, the incorporation of 1H-CBH into mixed-cation PSCs yields a remarkable enhancement in power conversion efficiency (PCE) from 21.18% to 23.59%. Moreover, the 1H-CBH-modified devices demonstrated exceptional environmental stability, retaining their initial morphology after 8 months under ambient conditions (25 ℃, 50-80% relative humidity), whereas unpassivated counterparts underwent complete degradation. Under inert N<sub>2</sub> atmosphere, PSCs incorporating 1H-CBH maintained >80% of their initial PCE after 600 h continuous storage. These results highlight the critical role of multifunctional additive engineering in achieving highly efficient and durable perovskite solar cells, paving the way toward scalable and reliable photovoltaic technologies.
- Research Article
- 10.3390/coatings16030293
- Feb 27, 2026
- Coatings
- Bin Ma + 4 more
In this paper, the regenerated NdFeB magnets were fabricated by Nd85Al15 alloy diffusion, and the influence of alloy content and diffusion temperature on the properties and microstructure was systematically studied. The recovery mechanism of magnetic properties was discussed based on the analyses using scanning electron microscope (SEM), energy dispersive spectrometer (EDS) and electron probe microanalysis (EPMA) observation. The results indicate that the coercivity (Hcj) increases significantly with both alloy addition and temperature, reaching the maximum value of 1087 kA/m (80.9% enhancement) compared with the non-diffused magnet (601 kA/m). The maximum remanence (Br) and maximum energy product (BHmax) of the diffused magnet are 0.99 T and 184.7 kJ/m3, which are 8.8% and 5.9% lower than those (1.085 T and 196.3 kJ/m3) of the non-diffused magnet. The density and compressive strength of the diffused magnet are enhanced by 8.2% (7.25 g/cm3) and 67.47% (628 MPa), respectively. As the compensation of Nd85Al15 melt, the density, Br and BHmax are improved via the liquid filling into pores. Simultaneously, the Hcj is enhanced through the repair of grain boundary defects and the formation of continuous Nd-rich phases.
- Research Article
- 10.1002/sstr.202500885
- Feb 27, 2026
- Small Structures
- Wei Fan + 13 more
Combining 2D and 3D perovskites has become a common strategy, and a range of methods for fabricating 2D/3D heterointerfaces jointly improve device performance and stability by grain boundary defect passivation and protective capping layer formation. Although more 1D and 0D perovskites are now considered for fabricating interfaces with 3D perovskites, 2D perovskites remain the most widely studied category, whose inorganic frameworks consist almost entirely of corner‐sharing octahedra. However, structurally distinct 2D perovskites, including those with face‐sharing inorganic octahedra which is a typical characteristic of 1D perovskites, have seldom been reported for integration with 3D perovskites to boost device performance and stability. Herein, we employ phenylethylammonium (PEA), phenylpropanylammonium (PPA), and 2‐phenoxyethylammonium (POEA) cations to fabricate LD/3D interfaces, where POEA facilitates an LD perovskite framework with both corner‐ and face‐sharing octahedra, thus enlarging grain size, optimizing surface potential for efficient carrier transport, stabilizing the n = 1 phase during thermal stress, and improving surface thermal conductivity. Consequently, POEA‐based perovskite solar cells (PSCs) with a bandgap of 1.53 eV delivered a champion power conversion efficiency (PCE) of 26.4%, demonstrating superior operational stability with 99% PCE retention after 180 h of maximum power point tracking.
- Research Article
- 10.1021/acsapm.5c04662
- Feb 24, 2026
- ACS Applied Polymer Materials
- Marvin Hoffer + 4 more
Torsional force spectroscopy is employed to probe the in-plane nanomechanical properties of solvent-annealed polystyrene-block-polybutadiene (SB) diblock copolymer films, which feature stiff polystyrene (PS) cylinders embedded in a softer polybutadiene (PB) matrix. By converting the torsional frequency shift and excitation amplitude into in-plane shear stress, storage shear modulus, and torsional dissipated energy, we map nanoscale variations in polymer-chain flexibility within three different defect structures. (1) An isolated ring defect reveals distinct direction-dependent shear behavior: when shear is applied perpendicular to the PS cylinder length axis, lower in-plane shear stress compared to parallel shearing indicates enhanced “wobbling” of the cylinders due to limited intramolecular resistance. (2) A previously unreported, sphere-like protrusion exhibits highly inhomogeneous in-plane shear stress yet nearly uniform dissipated energy, suggesting a swollen, mushroom-like PS cap structure connected to concealed PS cylinders beneath the surface. (3) Matrix dislocations and grain boundary defects show elevated in-plane shear stress and reduced dissipated energy at PS cylinder branching points, particularly at dislocation cores and grain boundary nodes, caused by chain compression and restricted flexibility. In contrast, bridging segments between the nodes exhibit lower in-plane shear stress and higher dissipated energy due to increased polymer-chain flexibility. These findings demonstrate that defect structures originating from local swelling, chain compression, and orientation mismatch introduce strong anisotropy into in-plane nanomechanical properties, offering pathways to tailor stiffness and flexibility in block copolymer-based nanotechnologies.
- Research Article
- 10.1002/aenm.202505854
- Feb 21, 2026
- Advanced Energy Materials
- You Gao + 19 more
ABSTRACT Non‐radiative recombination induced by grain boundary defects remains a critical challenge limiting the performance of perovskite solar cells (PSCs). This work proposes a dynamic passivation mechanism using molten 4‐phosphonobutyric acid (4‐PBA) during perovskite crystallization. Unlike solid‐state passivators, molten phosphonoalkanoic acid molecules penetrate deeply into bulk regions and access hidden defect sites that are otherwise unreachable. In the molten state, the phosphonic (─PO 3 H 2 ) and carboxylic (─COOH) groups exhibit high conformational freedom, enabling spontaneous rotation and optimal spatial alignment to match the atomic arrangement of perovskite defects. The butane chain in 4‐PBA creates an ideal separation of 5.4–7.7 Å between its ─PO 3 H 2 and ─COOH groups. This allows it to bridge the dual defects in adjacent [PbI 6 ] 4− octahedra, enabling cooperative dual‐site passivation. As a result, 1.68 eV wide‐bandgap PSCs employing this bulk‐doping strategy with the evaporation‐coating hybrid method achieve a power conversion efficiency (PCE) of 22.53% (certified 21.95%) and show minimal efficiency degradation over time, demonstrating robust operational stability.
- Research Article
- 10.1038/s41467-026-69524-8
- Feb 18, 2026
- Nature Communications
- Marleen Klann + 16 more
The diverse pigmentation patterns of animals are crucial for predation avoidance and behavioral display. This diversity arises from interactions among distinct pigment cell types, yet mechanisms generating pattern variation across teleost fishes remain incompletely understood. In zebrafish, Turing models have been proposed to explain stripe patterns, but it is unclear if they apply to other fishes. Here, we investigate the Snowflake mutant of the anemonefish Amphiprion ocellaris, which displays enlarged white bars with irregular boundaries. Using genome-wide association mapping and targeted sequencing, we identify a missense mutation (E42K) in gja5b, encoding the gap junction protein Connexin 41.8. CRISPR/Cas9-mediated genome editing recapitulates the Snowflake phenotype, while pharmacological inhibition of gap junctions phenocopies the boundary defects, supporting a causal role for impaired intercellular communication. Expression analyses reveal that, unlike zebrafish, anemonefish gja5b is predominantly expressed in iridophores. With functional in vitro assays we demonstrate that the E42K mutation acts as a dominant negative, strongly reducing gap junctional coupling. Introducing the same mutation in zebrafish reveals context-dependent effects on pigment patterning. Taken together our findings highlighting gap junction–mediated communication as a conserved but flexible mechanism controlling pigment boundary positioning and pattern diversification.
- Research Article
- 10.1088/1361-6501/ae412f
- Feb 13, 2026
- Measurement Science and Technology
- Li Zhang + 3 more
Abstract The dimensions of localized surface defects, e.g. width, length, and depth, significantly influence the vibration characteristics of bearings. Understanding the fault mechanism necessitates a dynamic model capable of accurately simulating these characteristics. Its accuracy heavily relies on the precise portrayal of the interaction between the ball and the defect boundaries within the model. However, most existing studies use pre-planned excitations, so neglecting the actual interaction dynamics between the ball and defective raceway. This paper proposes an improved model for defective bearings that considers interactions via the instantaneous positions of the ball and the three-dimensional defect area. It approximates the spatially dependent force deflection relationship using an artificial neural network, which characterizes ball-line contact between the ball and defect edges. This specific relationship cannot be described by a closed-form solution derived from classical contact theory. The validity and accuracy of proposed model are confirmed by comparisons with experimental responses from defective deep groove ball bearings. This study offers a solid quantitative basis for investigating the underlying mechanisms responsible for abrupt variations in contact force and the associated vibration characteristics due to localized surface defects. Its correlation between actual defect dimensions and vibration measurement characteristics has the potential to advance diagnostic and prognostic algorithms, as well as data augmentation for deep learning techniques.
- Research Article
- 10.1002/adfm.74393
- Feb 4, 2026
- Advanced Functional Materials
- Huchao Li + 10 more
ABSTRACT Organic single‐crystal field‐effect transistors (OSCFETs) are regarded as an ideal platform for investigating intrinsic charge transport behaviors and developing high‐performance organic electronic devices, thanks to their ordered molecular stacking and minimal grain boundary defects. However, conventional integration methods frequently introduce impurities that induce interface defects or crystal damage, significantly impairing charge transport efficiency‐a long‐standing limitation plaguing diverse organic semiconductors. To address this critical challenge, we propose a universal strategy for the integration of two‐dimensional (2D) organic single crystals with fluorinated polymer dielectrics. This approach synergistically combines an in‐house microspacing in‐air sublimation (MAS) growth technique with a gentle, damage‐free transfer process, effectively eliminating interfacial imperfections. The resulting high‐quality crystal‐dielectric interfaces enable OSCFETs to achieve exceptional comprehensive performance: a record‐high mobility of 18.9 cm 2 V −1 s −1 , ultralow operating voltage of −5 V, ultrafast photoresponse of 30 µs, outstanding high‐speed image acquisition capability, and robust dual‐mode driving performance for organic light‐emitting diodes (OLED). This work establishes a universal method for constructing high‐quality single crystals on polymer dielectrics, which holds broad implications for advancing high‐speed sensing, imaging technologies, flexible displays, and integrated logic circuits.
- Research Article
- 10.1002/smsc.202500288
- Feb 1, 2026
- Small science
- Dana M Stone + 10 more
Glasses derived from metal-organic frameworks (MOFs) combine the processing benefits of glassy materials with the accessible and selective porosity of MOFs, with potential applications in gas separation and electronics. Establishing control over MOF glasses requires an accurate understanding of how processing parameters will affect the resulting glass properties. To advance this understanding, the effect of isothermal melt treatment conditions on the porosity and morphology of ZIF-62 is investigated. It is demonstrated that the transition from crystal to glass increased in fractional free volume (3.78 ± 0.07% to 5.50 ± 0.03%, respectively) while impeding the accessibility of CO2, N2, and propene by 59-79%. It is demonstrated that the change in pore volume is independent of isothermal hold times. In contrast, isothermal hold time allows control over glass morphology, where short treatments retained more original morphological characteristics, while longer treatments improved grain coalescence.
- Research Article
1
- 10.1021/acsenergylett.6c00048
- Jan 30, 2026
- ACS Energy Letters
- Yulu Hua + 16 more
Large-area perovskite light-emitting diodes (LEDs) remain limited by severe performance losses arising from grain boundary defects and nonuniform film formation. Here we introduce a ZnBr2-mediated crystallization strategy that selectively passivates grain boundary defects while inducing the in situ formation of the wide-bandgap Cs2ZnBr4 interphase. This intergranular phase bridges adjacent CsPbBr3 grains, suppressing trap-assisted recombination, directing preferential crystal orientation, and enhancing environmental stability. Leveraging this approach, we realize large-area quasi-2D perovskite LEDs (active area: 225 mm2) exhibiting record-high external quantum efficiencies (EQEs) of 25.2% for green emission at 516 nm and 23.7% for red emission at 640 nm, which are the highest reported to date for devices of this scale. These results establish intergranular phase engineering as an effective and generalizable route to overcome intrinsic scaling challenges in quasi-2D perovskites, paving the way for efficient, stable, and manufacturable perovskite light-emitting technologies.
- Research Article
1
- 10.29130/dubited.1782087
- Jan 21, 2026
- Düzce Üniversitesi Bilim ve Teknoloji Dergisi
- Musa Doğruer
This study investigates the influence of CoFe2O4 (CFO) content variation (x = 0.000 to 0.010) on the mechanical, structural and superconducting properties of Bi-2223. Vickers microhardness measurements show a clear decrease in hardness with increasing CFO content. This decrease is linked to grain boundary weakening, structural defects, and impurity phases. Multiple hardness models are applied to analyze the indentation size effect (ISE). The Hays-Kendall model provided the closest fit to plateau region. SEM analysis reveals that higher CFO doping leads to increased grain fragmentation, irregular grain shapes, and reduced grain connectivity. Magnetization versus temperature (M–T) measurements are performed. The critical onset temperature (Tc) decreasing from 109.8 K (CFO-0) to 93.4 K (CFO-5) due to enhanced structural disorder and increased magnetic scattering. In summary, the study reveals that adding CFO leads to a decline in both mechanical and superconducting performance of the Bi-2223 samples. This is mainly because of increased grain boundary defects and magnetic scattering.
- Research Article
2
- 10.1021/acsami.5c23138
- Jan 21, 2026
- ACS applied materials & interfaces
- Xiyao Zhang + 2 more
Over the past decade, perovskite photovoltaics facilitated by solution-processed metal halide perovskites have garnered significant attention in both academic and industrial sectors. Studies demonstrated that device architecture plays a crucial role in the device-performance of perovskite photovoltaics. In this review, we summarize the evolution of device architectures of perovskite photovoltaics, mesoporous scaffold, planar heterojunction, and bulk heterojunction, centered on "core challenges driving structural evolution" as the main theme and driving momentum to develop an analytical framework that ties device architectures to charge transport, defects, and ion migration management. We outline these three device architectures using a template of "advantages - limitations - improvement paths" anchored in the three key dimensions: efficiency, stability, and scalability. We explicitly analyze both mesoporous scaffold and planar heterojunction device structures, particularly correlating device architecture with the core challenges for boosting and manufacturing perovskite photovoltaics. We describe the motivation for developing a bulk heterojunction. Afterward, we summarize the advantages of bulk heterojunction device structures through a controllable interpenetrating network with nanoscale phase separation, which enables local band microalignment, minority-carrier highways, Fermi-level repositioning, charge transport balancing, ion-migration restriction, and bulk/grain boundary defect passivation. Lastly, we envision future research focusing on the bulk heterojunction and providing a roadmap to guide scale-up and accelerate the commercialization of perovskite photovoltaics.
- Research Article
3
- 10.1002/adfm.202531852
- Jan 20, 2026
- Advanced Functional Materials
- Guodong Li + 8 more
ABSTRACT The excess of residual PbI 2 and the grain boundary defects in perovskite films limit the performance and stability of perovskite solar cells (PSCs). This study proposes a strategy for secondary phase transformation of residual PbI 2 and grain boundary encapsulation in perovskite films based on the 4‐pyridinecarboximidamide hydrochloride (4‐FAPyCl 2 ) additive. By introducing 4‐FAPyCl 2 into the PbI 2 precursor solution, a quasi‐2D perovskite coating of the grain boundaries was successfully constructed, achieving effective protection of the 3D α‐FAPbI 3 perovskite. This strategy not only significantly increases the perovskite grain size and eliminates pinholes but also promotes the formation of a 2D/3D heterojunction encapsulation structure at the grain boundaries, effectively passivating defects, suppressing non‐radiative recombination, and relieving residual stress. The optimized n‐i‐p planar PSCs achieved a champion power conversion efficiency (PCE) of 25.32 %. Besides, PSCs prepared under natural humid air conditions exhibit a PCE loss < 3 %. Meanwhile, due to the enhanced hydrophobicity and phase stability of optimized perovskite films, the PSCs exhibited excellent long‐term humidity environment storage, thermal, and light stability. This work provides an innovative idea for synergistically regulating the photoactive secondary phase of PbI 2 and constructing high‐performance 2D/3D perovskite structures, promoting the development of efficient and stable PSCs.