Achieving a simultaneous balance of cost, efficiency, and operational stability is critical for the commercial viability of perovskite photovoltaics. Planar-junction carbon-based perovskite solar modules (C-PSMs) represent a promising platform toward this goal, offering low-cost fabrication and long-term environmental stability enabled by thick carbon electrodes that eliminate the need for encapsulation. However, their power conversion efficiency remains fundamentally limited due to the discontinuous charge percolation and poor heterojunction contact at the carbon/perovskite junction. To overcome these challenges, we present a Holistic Anode Interface Design (H-AID) strategy that integrates two complementary approaches. First, a picosecond laser is used to sculpt a curved perovskite surface morphology, increasing contact area and enhancing charge transfer (Design-1). Second, a gallium-indium eutectic liquid metal is introduced into the carbon paste to fill internal voids and restore conductive pathways (Design-2). Their combination (Design-3) achieves a 42% improvement in module efficiency, reaching 16.88% over a 61.22 cm2 active area, among the highest reported for planar C-PSMs. Moreover, the device retains over 95% of its initial performance after 1200 h under ambient, encapsulated conditions. This work establishes a scalable H-AID framework to unlock cost-efficiency-stability co-optimization in carbon perovskite modules.
Buried interfacial imperfections between perovskite and hole-transport layer (HTL) represent a primary origin of non-radiative recombination and operational instability in inverted perovskite solar cells (PSCs). Incomplete self-assembled monolayers (SAM) coverage and inferior interfacial contact produce energetic disorder, hindering charge extraction to result in substantial photovoltage loss. Here, we introduce a bifunctional post-assembly interfacial reconstruction strategy employing 1-(2-hydroxyethyl) imidazole (2Hyimi) and 1,3-diaminopropane dihydroiodide (PDADI) to simultaneously improve both energy-level alignment for charge extraction and the wetting/nucleation environment at the HTL/perovskite interface during film formation. The amino groups in PDADI and the imidazole groups in 2Hyimi synergistically coordinate with residual and undercoordinated Pb2+ ions, effectively passivating buried interfacial traps, enhancing hole extraction and suppressing non-radiative recombination. Concurrently, the hydroxyl-terminated 2Hyimi improves surface wettability, promoting uniform crystallization and preferred orientation in large-area perovskite films. As a result, inverted PSCs achieve an efficiency of 26.46%, and perovskite solar modules with an active area of 51.50 cm2 reach 23.33%. Under ISOS-L-2 conditions, the target devices retain 92.29% of the initial efficiency after 1000 h at continuous maximum-power-point tracking, demonstrating excellent operational stability. This work establishes cooperative dual-molecular interfacial engineering as a scalable route to simultaneously enhance efficiency and stability in inverted perovskite photovoltaics.
Zn-based batteries are promising candidates for sustainable, large-scale energy storage. However, their practical deployment is hindered by dendritic Zn growth, parasitic side reactions and sluggish interfacial Zn2+ transport. Inspired by phospholipid membranes, we introduce a biomimetic zwitterionic hydrogel electrolyte (PAMC) to integrate 2-methacryloyloxyethyl phosphorylcholine, polyacrylamide and trace acrylic acid into a mechanically robust network featuring strong electrode adhesion and hierarchical Zn2+ pathways. The zwitterionic moieties regulate the primary Zn2+ solvation structure by partially replacing water ligands, thereby reducing the desolvation energy barriers and homogenize Zn2+ flux at the electrode interface. Consequently, PAMC delivers a high ionic conductivity of 44.94 mS cm-1 and a record Zn2+ transference number of 0.75, enabling dendrite-free Zn deposition and suppressed hydrogen evolution. Symmetric Zn||Zn cells exhibit stable cycling for over 2200 h, while Zn||Cu cells maintain highly reversible Zn plating/stripping for more than 2000 h. Furthermore, full cells with activated carbon, NaV3O8 and I2 cathodes demonstrate outstanding cycling stability and rate capability. When integrated with a perovskite solar cell, the Zn||I2 battery achieves an overall conversion efficiency of 13.3%, representing the highest reported to date for this category. This biomimetic electrolyte design establishes a universal platform for highly reversible Zn anodes and sustainable energy-storage systems.
Vertically inhomogeneous strain within perovskite crystalline layers remains a critical barrier to achieving high efficiency and long-term stability in perovskite solar cells. Herein, we address this challenge by integrating ascorbyl glucoside into hydrothermally synthesized TiO2 nanocrystals derived from TiCl4 to reduce the surface energy of TiO2 electron transport layer. The small surface energy establishes a liquid/solid/air interface, creating a dewetting effect to trigger stressed perovskite lattice at the bottom region. This design aligns with the liquid/air interface at the top, typically accompanied by formation of an inevitably strained top surface of the perovskite crystals. By precisely controlling crystallization dynamics of the liquid/solid/air interface, we successfully obtained a compressively strained perovskite film that is homogeneously strained throughout the out-of-plane direction. This uniform strain perovskite films deliver outstanding device performance, improving efficiencies to 25.34% of target from 23.20% of control for small-area devices (0.09 cm2), and 24.13% of target from 21.25% of control for large-area devices (1.00 cm2). Moreover, the optimized device demonstrate remarkable operational stability, retaining over 95% (T95) of its initial efficiency for over 2 000 h. The mechanically informed strategy introduces a new paradigm for strain engineering, offering valuable insights into the design of high performance perovskite photovoltaics.
Scalable manufacturing of perovskite solar cells is fundamentally limited by the vulnerability of perovskite crystallization to ambient moisture and oxygen, particularly during blade coating where an extended pre-annealing interval exposes unstable intermediates. Here, we introduce a surface-confined protection strategy to intrinsically stabilize perovskite film formation under ambient conditions. By introducing dipropylammonium trifluoroacetate (DPTA) into the perovskite precursor ink to spontaneously form a dense and self-assembled surface layer, selectively shielding the wet perovskite pre-film from environmental attack during the critical pre-annealing stage. This transient yet effective barrier preserves the PbI2·NMP intermediate to prevent pre-annealing degradation of the perovskite lattice even at high humidity. Simultaneously, the multifunctional ionic nature of DPTA allows strong coordination and hydrogen-bonding interactions with the perovskite lattice, leading to reduced bulk and interfacial defects. As a result, air-processed blade-coated MA-free perovskite solar cells reach an efficiency of 26.14% (certified at 25.75%), and retain 93.11% of the initial efficiency after 1300 h under continuous 1 sun illumination tested at maximum-power-point. The strategy readily translates to manufacturing-relevant perovskite solar modules, delivering 22.72%-efficiency on substrate area of 100 × 100 mm2. These results establish surface-confined protection as a general principle for scalable perovskite photovoltaics under ambient conditions.
Simultaneously addressing nanoscale interfacial charge transport inefficiency and Ag electrode diffusion remains a critical bottleneck for scalable inverted perovskite solar cells (PSCs). Herein, we report a dual-functional molecular engineering strategy by doping 2-mercaptopyridine-N-oxide (2-MPNO) into the 10 nm-thick nanoscale bathocuproine (BCP) cathode buffer layer, achieving synergistic optimization of interfacial energy alignment and Ag+diffusion inhibition. The ntype doping effect of 2-MPNO triples the electron mobility of the [6,6]-phenyl-C61-butyric acid methyl ester (PCBM)/BCP layer (via space-charge-limited current measurements), with ultraviolet photoelectron spectroscopy confirming a 0.37 eV upward Fermi level shift to optimize nanoscale interfacial energy alignment. Owing to the incomplete coverage of PCBM on the perovskite surface, 2-MPNO molecules infiltrate the perovskite interface, effectively passivating defects and reducing non-radiative recombination. Concurrently, the-SH and N-O groups of 2-MPNO form bidentate coordination with Ag at the nanoscale Ag/BCP interface, constructing a molecular barrier to block Ag+ migration. As a result, the optimized device exhibits an improvement in efficiency from 23.56% to 25.31%. More importantly, unencapsulated devices maintain 97.4% of their original efficiency after 2115 h stored in air with a relative humidity of 15% +/- 5% and retain 94.0% of their initial efficiency following thermal aging at 65 degrees C for 1256 h in a nitrogen environment.
The buried interface between electron transport layer (ETL) and perovskite absorber often induce the awful properties of perovskite film such as interfacial defects, trenched structure and ion migration, hindering improving efficiency and stability of perovskite solar cells (PSCs). Here, we present a multiscale planarized interface regulation (MPIR) strategy by introducing it-conjugated zero-dimensional (0D) metal halide, BPP2MnBr4 (BPP+ = C25H22P+), as multifunctional interlayer on SnO2. The it-conjugated multi-phenyl framework enables strong coupling with adjacent functional layers, while the 0D configuration provides quantum confinement and structural robustness. Theoretical and experimental analyses reveal that BPP2MnBr4 increases the formation energy of non-photovoltaic phase (delta-FAPbI3), thus improving phase purity. Additionally, buried interface modified by BPP2MnBr4 flattens grain boundary trenches to release residual stress for perovskite film. Benefiting from MPIR achieves a high efficiency of 25.88 %, and good stability for maintaining 92.0 % of initial efficiency after 1000 h of continuous light irradiation in N2 without encapsulation of perovskite devices. Besides, the resulted solar module with an active area of 25.74 cm2 (6.5 cm x 6.5 cm x 9 sub-cells) exhibits a PCE of 22.37 % with excellent uniformity. These results establish it-conjugated 0D metal halides as multifunctional interlayers capable of simultaneously improving structural robustness and operational reliability in perovskite photovoltaics.
Organic-inorganic perovskite materials face challenges related to the presence of non-neutralized charge centers, such as positively charged local defects arising from lattice imperfections like point-vacancies and under-coordinated lead ions at lattice edges, hindering their photoelectric intrinsic properties. We introduce 3,3-difluoropyrrolidine hydrochloride (GOSO-005), a novel dipolar molecule, as an effective solution for neutralizing positive charge centers within perovskites. GOSO-005, with its high dipole moment and fluorinated groups, interacts with charged defects to neutralize them, thus reducing defect density and minimizing the effective electron-capturing radius. This neutralizing strategy enhances charge transport, reduces Shockley-Read-Hall recombination, and boosts an impressive efficiency of 26.09% (certified 26.12%) for perovskite solar cells. In parallel, the fluorinated dipolar molecule introduces additional hydrophobicity to the resultant perovskite, thereby significantly enhancing the long-term environmental, continuous illumination operational, and thermal stabilities of the perovskite solar cells.
Chirality transfer from molecules to supramolecular architectures underpins diverse biological and material functions, yet constructing helical heterojunctions remains a formidable challenge. Here, we report the discovery of nanoscale helical junctions directed by a molecular chiral junction derived from a meso-form lipid emitter with two heterochiral centers. Unlike enantiopure molecules, which assemble into uniform homochiral fibers, the meso-form molecule self-assembles into planar belts in pure DMSO and striking helical heterojunctions with opposite-handed portions in DMSO/H2O 9:1 (v/v). Spectroscopic and structural analyses reveal that solvent polarity and stereochemical configuration govern distinct packing modes and hierarchical chirality amplification. This unprecedented molecular-to-supramolecular transformation provides a new paradigm for chirality engineering, offering mechanistic insights into chiral self-assembly and opening opportunities for advanced chiroptical materials.
Defects at the buried interface represent a critical challenge that impedes further improvements in both the performance and scalable manufacturing of perovskite solar cells (PSCs). Defect formation, lattice mismatch, and energy-level misalignment at this interface aggravate nonradiative recombination and accelerate photothermal degradation, thereby limiting both efficiency and operational stability. Here, we employ interface engineering using multifunctional molecules to suppress defect formation. To minimize redundant material screening, we combine theoretical calculations with experimental validation to identify 4-aminobutylphosphonic acid (4-ABPA) for modifying the interface between the perovskite layer and the electrode. Both simulation and experimental results demonstrate 4-ABPA as a multifunctional molecular bridge that simultaneously anchors to the charge transport layer and interacts with the perovskite lattice. And its role in dynamically regulating perovskite crystallization and enhancing interfacial performance is uncovered. The dual-site chemical binding regulates crystallization, alleviates residual stress, suppresses interfacial defects, and optimizes energy-level alignment at the buried interface. As a result, voltage loss is reduced to 31 mV, enabling power conversion efficiencies of 25.56% in n-i-p and 26.45% in p-i-n architectures with negligible hysteresis. The modified devices also exhibit outstanding durability, retaining 83.91% of their initial performance under 1440 h of continuous operation and 91.59% after 2600 h of ambient storage. Our work establishes a systematic and universal buried-interface engineering strategy to further enhance efficiency and stability, thereby advancing the mass production of perovskite devices.
Self-assembled monolayers (SAMs) are critical for high-efficiency inverted perovskite solar cells (PSCs), but their use is limited by incomplete coverage, weak oxide adhesion, solvent desorption, and poor wettability. These issues stem from a structural constraint: conventional SAMs anchor through a single monodentate "hinge," whose rotation hinders dense packing, creates surface-energy heterogeneity, and destabilizes bottom and buried interfaces. Here, we introduce a molecular-interlock strategy by incorporating lactic acid (LA) to pair with Me-4PACz to restrict this rotational freedom. The carboxyl group of LA forms an additional coordination with hydroxylated NiOx and simultaneously interacts with undercoordinated Pb-I species at the buried perovskite interface, creating a dual-anchor configuration that enhances SAM adhesion and structural rigidity. This interlocked SAM improves surface uniformity, increases wettability toward perovskite inks, suppresses PbI2-related defect formation, optimizes energy-level alignment, and releases interfacial residual stress, enabling compact and pinhole-free perovskite films. As a result, PSCs using Me-4PACz (LA) achieve a PCE of 26.87% (certified 26.31%), maintain 98.8% of their initial output after 1000 h MPP tracking, and retain 90% efficiency after 1200 h ambient storage. Large-area (47.84 cm2) modules reach 23.18%, demonstrating the broad applicability of rotationally restricted, molecular-interlocked SAMs for robust and efficient perovskite photovoltaics.
Flexible perovskite photovoltaics have reached impressive laboratory efficiencies, but their path toward industrial reality remains fragmented. Conventional fabrication approaches treat chemistry and mechanics as independent variables, overlooking the fact that crystallization in roll-to-roll (R2R) processes occurs under continuous shear, substrate tension, and spatiotemporally varying evaporation fields. This Perspective proposes a chemical-mechanical co-design framework in which precursor solvation chemistry, ink rheology, and coating hydrodynamics are engineered as a coupled system. We discuss how mechanical fields such as shear strain, meniscus forces, and substrate bending, actively modulate nucleation, intermediate phase evolution, and stress relaxation. We further compatible with high-speed slot-die coating. Finally, we outline how intelligent manufacturing, integrated sensing, and AI-assisted control can converge to unlock mechanically compliant, highly uniform, and truly scalable flexible perovskite modules.
This study addresses the inherently low damping and vibration susceptibility of carbon fiber reinforced polymer (CFRP) laminated cantilever plates by developing a comprehensive dynamic modeling and active vibration control framework. An electromechanical coupling model incorporating macro-fiber composite (MFC) actuators and sensors is established using the first-order shear deformation theory (FSDT) and the assumed mode method, with virtual springs introduced to account for non-ideal clamped boundary conditions. A reduced-order state-space model is then derived through model reduction, and a linear quadratic Gaussian (LQG) controller is designed for optimal state estimation and feedback control. The theoretical model is systematically validated via convergence analysis, ANSYS finite element simulations, and LMS impact hammer testing. The results demonstrate that, with the relative errors of the first four natural frequencies controlled within 2%, the theoretical mode shapes are highly consistent with those obtained from ANSYS simulations. An active vibration control experimental platform is established, and the effectiveness of the control strategy is verified under dual-spectrum harmonic and impact excitations. The results show that the designed LQG controller can effectively suppress multi-modal vibrations, substantially attenuating the response amplitudes of dominant modes and significantly accelerating the transient vibration convergence. This study addresses the challenge of precisely characterizing actual non-ideal clamped boundary conditions. Through model order reduction and closed-loop LQG control experiments, it provides a comprehensive set of theoretical methodologies, numerical solution strategies, and engineering-oriented experimental schemes for the electromechanical coupling dynamic modeling and optimal vibration suppression of CFRP thin-walled composite structures.
The electron transport layer (ETL) is widely recognized as a critical component in perovskite solar cells (PSCs), as it modulates the efficiency of charge extraction and transport processes, which largely dictates the overall device performance.In this study, we incorporated cysteine-functionalized silver selenide quantum dots (Cys-Ag2Se QDs) into the SnO2 ETL to establish efficient electron transport pathways. The introduction of Cys-Ag2Se QDs effectively modulated the optoelectronic properties of SnO2, including carrier mobility, conductivity, and energy level alignment. Furthermore, the Cys-Ag2Se QD-modified SnO2 ETL regulated perovskite crystallization dynamics, yielding perovskite film with enlarged grain sizes and improved quality. Notably, the Cys-Ag2Se QDs exhibited remarkable stress-relieving properties at the buried interface due to their nanoscale curvature and ligand interactions, mitigating residual lattice strain and enhancing interfacial integrity and long-term stability. Additionally, the Cys-Ag2Se QDs passivated uncoordinated Sn4+ and Pb2+ defects at the SnO2/perovskite interface, reducing trap-state density and suppressing non-radiative recombination. The optimized device (0.03 mg/mL Cys-Ag2Se QDs) achieved a champion power conversion efficiency (PCE) of 23.42%, with enhanced short-circuit current density (Jsc) and fill factor (FF). After 1000 h of continuous heating at 60 degrees C under nitrogen, the Cys-Ag2Se incorporated PSCs retained 90.54% of their initial efficiency. This work presents a facile fabrication strategy and a novel QD-based additive system for high-performance SnO2 ETLs in PSCs.
Poly(vinylidene fluoride) (PVDF)-based solid electrolytes represent a compelling frontier for solid-state lithium metal batteries. Unfortunately, their practical implementation is severely impeded by high Li+ migration energy barrier and pronounced interfacial instabilities, arising from α-phase-rich conformations and undesired Li+-solvation environments. In this study, an 'all-in-one' regulation strategy enabled by N-methylimidazolium bis((trifluoromethyl)sulfonyl)imide (MimTFSI) is proposed, which synergistically engineers a β-phase polymer matrix for shortened pathways and constructs an anion-rich solvation sheath for lowered energy barriers, ultimately unlocking fast and stable Li+ transport coupled with exceptional interfacial compatibility. Consequently, this integrated solid-state electrolyte demonstrates a high ionic conductivity of 0.84 mS cm- 1, supports stable cycling of Li symmetric cells for over 4000 h at 0.1 mA cm- 2, and delivers outstanding cycling performance in Li/LiNi0.8Co0.1Mn0.1O2 full cells, retaining 93.8% of its initial capacity after 930 cycles at 0.5 C and 95% over 500 cycles at 1 C. Even under expanded voltage windows, it retains 80% after 580 cycles at 4.4 V and 84% after 160 cycles at 4.5 V. Furthermore, the pouch cell is capable of delivering a discharge capacity of 3.26 mAh cm-2, demonstrating the strong applicability for next-generation solid-state lithium metal batteries.
Realizing high-performance perovskite/silicon tandem solar cells requires precise control of wide-bandgap perovskite crystallization. Solvent engineering is the most direct lever for this task; yet, its intricate, multi-variable mechanisms defy intuition-driven design. Herein, we overcome this bottleneck by pioneering a retrieval-augmented large language model to screen > 8000 solvents, identifying γ-valerolactone (GVL) as a non-toxic, high-performance cosolvent. It is found that the GVL strongly coordinates FA+, thus precisely modulating crystallization kinetics, retarding nucleation, and promoting oriented, micrometer-scale grain growth. The resulting films exhibit not only superior crystallinity, reduced non-radiative recombination, but also improved scalability to large area and the tolerance to increased film thickness. Consequently, both the single-junction and tandem devices achieve efficiencies of 23.3
Self-assembled monolayer (SAM)-based inverted perovskite solar cells (PSCs) suffer from a persistent efficiency-stability trade-off issue, which limits their commercialization. Herein, we propose a synergistic stabilizing strategy using reduced glutathione (GSH) as a multifunctional additive, integrating dipole modulation and redox-driven self-healing. GSH enables cross-scale regulation: inducing interfacial dipole via a concentration gradient, passivating bulk defects through Pb2+ coordination, optimizing crystallization kinetics, providing chemical protection against O2•- and moisture, and establishing a GSH/oxidized glutathione (GSSG)-Ni2+/Ni3+ redox cycle for self-healing at the NiOx/SAM interface. Moreover, the interaction between GSSG and NiOx opens an additional hole transport channel, effectively suppressing device performance degradation induced by ultraviolet (UV) irradiation and thermally-triggered cleavage of hydroxy groups in the SAM. Benefiting from the aforementioned advantages endowed by GSH, the small-area cell (4 mm2) achieved a high efficiency of 26.17%, while the 12.50 cm2 minimodule reached 23.14%-among the highest values reported for modules with comparable active areas. Target devices also exhibit exceptional ISOS (International Summit on Organic Photovoltaic Stability) protocols stability: retaining 69.8% (ISOS-T-1, 200 h), 91.0% (ISOS-D-1, 1056 h), and 78.44% (ISOS-L-2, 336 h) of their initial efficiency. This work breaks the efficiency-stability trade-off and offers a "dynamic regulation-static protection" design principle for PSCs.
ABSTRACT Defects in electron transport layers (ETLs) critically limit the performance of perovskite solar cells, particularly in flexible architectures. Here, we introduce a defect healing strategy using multifunctional carboxylic acids to modify SnO 2 ETLs on flexible substrates. Theoretical calculations reveal strong adsorption energies between carboxylate groups and SnO 2 surface atoms, enabling effective coordination with undercoordinated Sn sites and oxygen vacancies. Density functional theory screens that 2‐bromo‐1,3,5‐benzenetricarboxylic acid (BBA) exhibits the highest binding energy owing to synergistic Sn–Br interactions, which enhance interfacial coupling and electron transfer. The optimized interface between SnO 2 and BBA facilitates uniform perovskite film growth and suppresses trap‐assisted recombination. Consequently, the carbon‐based flexible perovskite solar cells deliver an efficiency of 17.07% and retain 68% of the initial efficiency after 30 days without encapsulation. This work establishes a versatile and low‐temperature strategy for defect regulation in SnO 2 ETLs, offering a promising pathway toward efficient and durable flexible perovskite photovoltaics.