Scalable fabrication of perovskite solar modules is hindered by processing inconsistencies and moisture-induced degradation. Although classic coordination solvents form thermodynamically stable intermediate phases with lead iodide (PbI2) under inert gas atmospheres, they are highly hygroscopic in ambient conditions. Moreover, due to minimal entropy change, this phase is difficult to remove during annealing, leading to micropores and unwanted phases. Here we introduce an enthalpy–entropy competition strategy for scalable, humidity-tolerant perovskite printing, in which dimethyl sulfoxide/N-methylpyrrolidone is replaced by N-butylpyrrolidone. N-butylpyrrolidone forms strong carbonyl–PbI2 coordination at ambient temperatures (enthalpy-driven), yet readily dissociates on heating (entropy-driven), facilitating easier formamidinium iodide embedding and intermediate-phase protection. The strategy yields perovskite solar modules with certified power conversion efficiencies of 23.97% in a 100-cm2 rigid module and 19.71% in a flexible counterpart. Encapsulated devices retain 80% of initial performance after 1,440 hours under the double 85 condition (85 °C, 85% relative humidity), demonstrating outstanding operational durability. By designing a solvent around enthalpy–entropy competition, the trade-off between film quality and humidity tolerance in perovskite solar module fabrication is overcome. The resulting 100-cm2 modules deliver certified efficiencies above 24% while maintaining excellent stability under harsh ageing conditions.

Here, a donor-acceptor integrated polymer, PQIC, featuring a rigid π-conjugated framework, is reported, in which a Y-type small-molecule acceptor is covalently fused into a polymer donor backbone. PQIC exhibits balanced bipolar charge transport, reduced defect density, and high electroluminescence efficiency. When incorporated as a third component, it facilitates charge percolation, concurrently weakens electron-phonon coupling and lowers defect-state density, thereby alleviating recombination losses. As a result, PQIC-based ternary organic solar cells achieve a power conversion efficiency of 20.81% (third-party certified at 20.60%). In addition to high efficiency, the devices exhibit excellent stability, thick-film tolerance, and scalability, retaining ~85% of their initial efficiency after 2000 hours of maximum power point tracking, delivering 19.11% with a 300-nanometer-thick active layer, and reaching 19.78% for 1-square centimeter devices. These results highlight the potential of PQIC-based ternary systems for advancing organic solar cells.

Two-dimensional (2D) perovskites are widely introduced into formamidinium (FA+) based three-dimensional (3D) perovskites due to their major benefits of: (i) stabilizing the α-phase of FA+-based perovskites; (ii) regulating the crystallization process; (iii) mitigating interface defects. However, knowledge regarding how the configuration of bulky ammonium cations influences the formation and performance of 2D/3D heterogeneous structures are still scarce. Here, we report that substituting phenethylammonium with methoxyl (MeO-PEA+) can decrease its solubility in polar solvents and enhance the α-phase stability for both the FA-based perovskite crystallization nuclei and final polycrystalline films. Adding a minimal concentration (0.3%) of p-methoxyphenethylammonium chloride (MeO-PEACl) in the perovskite precursor can achieve both a grain boundary wrapping and an in situ formation of buried 2D/3D perovskite structures, leading to solar cells with increased open-circuit voltage from 1.11 to 1.16 V and power conversion efficiency (PCE) from 21.1% to 23.1%. The resulting 2D/3D heterogeneous film can maintain its black phase after 3380 h of exposure at 65 ± 10% relative humidity, and the corresponding solar cells preserved 98% of their initial PCE after 1850 h of heating at 65°C.

Organic solar cells are attractive for wearable electronics, in particular, all-polymer solar cells (all-PSCs) offer superior intrinsic stability and higher output voltage, enabling direct matching with the energy storage and conversion systems. However, all-PSCs typically suffer from disordered morphology and poor donor-acceptor compatibility, requiring processing additives that compromise long-term stability. Here, we introduce a structural homology strategy, using donor and acceptor polymers that share the same bithiophene imide building block, to eliminate the need for additives. This design strengthens intermolecular interactions, enhances molecular ordering, and suppresses energy loss, yielding an open-circuit voltage of 0.94 V, a 12% improvement over the benchmark PM6:Y6 system. The chemical homology also reduces the Flory-Huggins interaction parameter and improves donor-acceptor compatibility, allowing the active layer to spontaneously form an ideal nanoscale fibrillar interpenetrating network. The resulting additive-free all-PSCs achieve a record power conversion efficiency of 19.12%, together with exceptional thermal stability (T80  =  1128 h), photostability (T80  = 756 h), and mechanical robustness. By integrating a 70 cm2 large-area all-polymer module with series-connected zinc-air batteries, we demonstrate a self-sustaining, solar-rechargeable system that delivers continuous power under both illumination and darkness, offering a practical pathway for next-generation flexible and wearable electronics.

ABSTRACT Low‐potential aldehyde oxidation offers an energy‐efficient anodic alternative to oxygen evolution for bipolar hydrogen production coupled with biomass valorization, yet the tandem non‐Faradaic/Faradaic mechanism remains poorly understood. Here, we report PtCu 3 ‐coated Cu nanowire arrays supported on Cu foam (PtCu 3 @Cu/CF) fabricated via galvanic replacement and electrochemical reduction. In situ ATR‐FTIR and DFT calculations indicate the PtCu 3 shell enhances adsorption of the gem ‐diolate intermediate while weakens binding of 5‐hydroxymethyl‐2‐furancarboxylic acid (HMFCA), accelerating both non‐Faradaic C–H cleavage and Faradaic oxidation. This enables selective 5‐hydroxymethylfurfural upgrading with anodic hydrogen evolution at 300 mA cm −2 at ∼0.21 V in a two‐electrode flow electrolyzer. Additionally, the electrolyzer also achieves 100 mA cm −2 at 0.16 V with 200% combined Faradaic efficiency for bipolar hydrogen production. Integration of a six‐cell stack with perovskite photovoltaic module yields a bias‐free solar‐to‐hydrogen efficiency of 16.9% alongside gram‐scale HMFCA production. This noble‐metal‐lean platform establishes scalable solar reforming for co‐generating green hydrogen and value‐added chemicals.

Single-component organic solar cells (SCOSCs) possess unique advantages in stability over multi-component ones (MCOSCs), yet their development in large-area blade-coating and flexible devices has progressed slowly, hampered by the typical trade-offs among efficiency, non-halogenated-solvent processability, and mechanical flexibility. Herein, we innovatively developed a new type of non-fully conjugated block copolymer (NF-CBC) PM6-b-PYIT-A with intrinsic non-halogenated-solvent-processability and mechanical robustness by integrating the strategy of synthesizing CBC via covalent linkage with flexible-moiety incorporation into the CBC backbone. Benefiting from suppressed aggregation behavior and extended nucleation/growth time, PM6-b-PYIT-5A exhibits superior compatibility with the broadened non-halogenated-solvent processing window. In contrast to the typical efficiency loss in the MCOSCs, the new NF-CBC PM6-b-PYIT-5A with flexible moiety achieved record power conversion efficiencies (PCEs) of 13.36% for small-area spin-coating devices and 12.05% for large-area blade-coating devices processed with non-halogenated solvents instead, significantly outperforming the reference PM6-b-PYIT with fully rigid backbones (12.80% and 10.60%). Moreover, the flexible moiety creates a better stress-dissipation system, enabling outstanding stretchability with 80% PCE retention at 40.39% strain for PM6-b-PYIT-5A, far surpassing PM6-b-PYIT (22.46%). This work demonstrates that the synthetic strategy for NF-CBCs, coupled with non-halogenated-solvent processing, triggers a pronounced performance reversal in SCOSCs, thus harnessing the flexible moiety to enable high-performance, large-area, stretchable SCOSCs.

Crystallographic defects and impurities dominating non-radiative recombination hinder the performance and reproducibility of large-area perovskite photovoltaics, especially in flexible application scenarios. Herein, a strategy is proposed for defect in situ detection and laser-based repair of large-area perovskite films. The regions with high density of crystallographic defects and impurities are identified and visually depicted by photoluminescence quantum yields and Urbach energy measurements, respectively. Moreover, the laser with a wavelength of 450 nm is employed to precisely and rapidly repair the regions, resulting in a significant reduction of defect content within the repaired perovskite film compared with the pristine one. Consequently, the champion power conversion efficiency (PCE) of 25.21% (certified efficiency of 24.57%) and 17.36% are achieved based on 1.01 cm2 flexible perovskite solar cells (PSCs) and 100 cm2 flexible solar modules, respectively, as well as a high yield rate of 90%. This work provides both technical and theoretical references for the commercialization of flexible perovskite photovoltaics.

The performance of perovskite photovoltaics is critically governed by the buried interface quality. Conventional interfacial layers, such as self-assembled monolayers (SAMs), often suffer from molecular aggregation, which compromises adhesion and promotes ion migration. To overcome this limitation, we introduce a dynamic anchoring molecular bridge, 6-aminohexylphosphonic acid hydrochloride (AHPH). Its dual-anchoring groups suppress SAM aggregation, while unbound molecules migrate during crystallization to guide the in situ formation of a low-dimensional perovskite heterojunction. This bridge robustly connects the charge transport layer to the perovskite bulk, enhancing mechanical stability and concurrently suppressing halide/lead ion diffusion. Furthermore, AHPH templates perovskite crystallization, improving film quality through nucleation control and Ostwald ripening. This synergistic interfacial engineering strategy, centered on constructing a dynamic molecular bridge for a robust buried heterojunction, enables inverted perovskite solar cells with a champion efficiency of 25.7% and significantly improved operational stability.

The operational instability of metal halide perovskites stems from an intrinsic coupling between lattice distortion, carrier localization and fatigue under cyclic stress. Here we report an entropy-engineered chiral heterointerface strategy that disrupts this degradation pathway. A trifluoromethyl-substituted chiral spacer cation is introduced at the buried interface to construct a low-dimensional heterostructure with enhanced dipolar interactions. The resulting heterointerface homogenizes the electrostatic potential, suppresses localized electronic states and relaxes the orientational constraints of formamidinium cations, thereby increasing configurational entropy and enhancing lattice adaptability under repeated illumination, thermal and electrical stresses. Together with chiral-induced spin-selective transport, this strategy promotes carrier delocalization, efficient charge extraction and spatially uniform recombination. Target device achieves a power conversion efficiency of 26.91% and retains 91.3% of their initial efficiency after 1,400 h of maximum power point tracking. This work establishes entropy engineering as a general framework for designing fatigue-resistant perovskite photovoltaics.

The chemistry of buried interfaces critically dictates the crystallization behavior of perovskite semiconductors in inverted perovskite solar cells, yet remains poorly controlled, giving rise to interfacial coordination disorder that disrupts the organization of self-assembled monolayers (SAMs) during crystallization. Here, we report an N-heterocycle-activated coordination strategy that stabilizes SAM organization while enabling precise regulation of precursor chemistry and crystallization at SAM-perovskite interfaces. Imidazolium-derived molecules integrated into SAMs establish cooperative coordination interactions with neighbouring lead polyhalide species, thereby reshaping the local precursor environment and directing nucleation and crystal growth. This process gives rise to a π-cooperative coordination interaction at the buried interface, which suppresses interfacial grooves and voids, reduces residual solvent-complex intermediates, and promotes the direct formation of phase-pure α-perovskite films. Devices based on this molecularly regulated interface achieve a power conversion efficiency of 26.83% and retain 93.8% of their initial efficiency after 936 h of continuous maximum power point operation. These results establish coordination-mediated interfacial design as a molecular route to couple interfacial order with crystallization control in perovskite semiconductors.

Advancing flexible and sustainable energy technologies requires photovoltaic systems that couple high efficiency with mechanical robustness and a minimized environmental footprint. Ultra-thin perovskite photovoltaics deliver exceptional specific power, yet their deployment is constrained by the lack of sustainable substrates with both mechanical durability under extreme bending. Here, we report a modified bamboo-derived cellulose vitrimer substrate paired with a permeable interfacial network formed from self-polymerizing ammonium salts. These dynamic multicovalent networks mitigate strain-induced interfacial degradation, thereby enabling mechanically robust operation under large strain. Ultra-thin perovskite photovoltaics fabricated on this platform achieve a champion efficiency of 23.27% and a specific power of 35 W/g, ranking among the highest values reported for ultra-thin photovoltaics. Notably, the devices maintain 91% of their initial efficiency after 15 000 bending cycles at a 1 mm curvature radius, while the cellulose substrate enables closed-loop recyclability under mild conditions. This work establishes a scalable and eco-conscious pathway to high-performance, mechanically robust perovskite photovoltaics, underscoring how dynamic multicovalent network design can advance sustainable, portable, and wearable energy technologies.

Geant4 (version 11.3.2) simulations were used to study particle-dependent radiation interaction in MAPbI3 under electron, photon, and neutron irradiation. The analysis focused on spatial distributions of interaction events, released energy, secondary-particle generation, and process-specific contributions. A 1 mm single-layer MAPbI3 target was used to identify the intrinsic material response, while multilayer MAPbI3 containing detector geometries were considered to assess device-like effects. Electrons produced extended charged particle tracks governed by direct energy loss and secondary-electron cascades. Photons showed weak direct energy deposition, with the response mainly controlled by secondary electrons generated in discrete electromagnetic interactions. Neutrons produced sparse but locally intense energy-release patterns dominated by recoil particles and nuclear-reaction products. The results show that total released energy alone is insufficient to describe radiation response in MAPbI3; spatial morphology and the balance between primary and secondary contributions are essential for interpreting both detector operation and possible radiation-induced degradation.

Metal halide perovskites have attracted significant attention as emerging semiconductors for low-dose X-ray detection. Their high atomic number elements, strong absorption, and long carrier diffusion lengths make them promising for medical imaging applications. This review highlights how advances in nanoscale science and nanotechnology are reshaping perovskite-based X-ray detectors. We discuss the influence of dimensionality, defect control, and interface engineering on charge generation and transport, together with the role of nanomanufacturing strategies such as confined crystallization and scalable printing. Recent progress in nanoscale characterization provides insight into carrier dynamics and stability, enabling a deeper understanding of low-dose operation. Finally, we outline forward-looking opportunities in flexible and wearable devices, integration with medical systems, and the development of sustainable materials. By framing perovskite X-ray detection within the broader context of nanoscience, we emphasize its potential to deliver efficient, reliable, and transformative platforms for future medical imaging.

Controlling the aggregation behavior of conjugated polymers is crucial for optimizing the morphology and performance of all-polymer solar cells (all-PSCs), yet achieving precise regulation remains a formidable challenge due to the complex self-assembly of polymers in solution. Herein, we report a series of bithiophene imide-based terpolymer donors (OH1 to OH4) with systematically increased thiophene pi-bridge content to modulate solution-state aggregation. Increasing the pi-bridge content progressively enhances aggregation, leading to improved molecular ordering and a favorable fibrous network morphology in blend films. The optimized OH4:PY-IT blend achieves a remarkable power conversion efficiency (PCE) of 19.25% in binary all-PSCs-among the highest reported to date. Moreover, both intrinsically stretchable and flexible devices based on OH4:PY-IT exhibit superior mechanical durability, retaining 85.3% of initial PCE after 200 deformation cycles under 10% strain and 80.1% after 7000 bending cycles, while achieving high PCEs of 14.47% and 15.63%, respectively. This work establishes pi-bridge main chain engineering as a powerful strategy to control polymer aggregation and morphology, providing key insights for developing efficient and mechanically robust all-PSCs.

Organic-inorganic halide perovskite solar cells (PSCs) have demonstrated a promising advancement in flexible and lightweight photovoltaics. Nevertheless, achieving their large-area printed fabrication remains challenging, especially the issue of defect enrichment at the buried interfaces, which is crucial for efficient carrier transport. Herein, an interfacial fastening strategy is designed to enhance the performance and stability of PSCs, involving the introduction of hexamethylene diisocyanate (HDI) into the perovskite precursor and ethylene glycol (EG) on electron transport layers. The in situ reaction between HDI and EG during film formation can inhibit the formation of complex intermediate phases during precursor deposition, thus achieving the uniform colloidal distribution, mitigating the gradient residual stress mismatch of perovskite films, and enhancing the buried interfacial contact. The resulting rigid, flexible PSCs and modules (25 cm2) achieve PCEs of 26.04%, 24.16%, and 20.40%, respectively, and encapsulated devices can retain over 80% efficiencies after storage for 6380 h. This work provides a potential to simultaneously optimize the contact quality at the buried interface and the crystallization quality of perovskites, which aligns with the requirements for large-area, high-quality, and homogeneous deposition of perovskite photovoltaics and facilitates the advancement of their printing manufacturing and commercialization transition.

The aging dynamics of perovskite precursor solutions critically govern the photovoltaic performance of solar cells. However, the underlying degradation mechanisms in low-dimensional perovskite precursors remain elusive, particularly regarding the pivotal role of spacer cations in modulating decomposition pathways. This study elucidates the intrinsic aging mechanisms in low-dimensional perovskite precursors, revealing that spacer cation integration fundamentally governs decomposition kinetics. A dual-functional solution stabilizer, 4-carboxy-2-fluorophenylboronic acid (CFB), is strategically designed to concurrently mitigate precursor degradation and regulate crystallization dynamics. The carboxyl moiety undergoes spontaneous deprotonation to establish robust hydrogen bonds with guanidinium (GA+), effectively suppressing methylamine (MA0)-mediated nucleophilic attacks and preventing irreversible addition-elimination reactions between GA+ and MA0. Simultaneously, CFB orchestrates multi-stage crystallization control through coordination modulation, yielding highly oriented perovskite crystals with passivated grain boundaries. The optimized devices demonstrate exceptional photovoltaic performance with a remarkably low energy loss of 0.38 eV. Notably, devices fabricated from aged precursors maintain 90% of initial efficiency over 42 days of ambient storage. Furthermore, unencapsulated devices deliver optimized humidity stability and thermal stability.

Solving the interfacial stability of perovskite solar cells (PSCs) is an inevitable requirement to achieve their long-term stability as well as commercial applications. Low-dimensional/three-dimensional perovskite heterojunctions (1D/3D or 2D/3D) have emerged as a promising architecture for efficient PSCs. Here, symmetric sulfonium-based molecules with tunable alkyl spacers are introduced to construct a heterojunction buried interface, achieving atomic-scale lattice matching between the perovskite film and the adjacent layer underneath. The interface, based on a one-dimensional (1D) spacer molecule with suitable steric hindrance and characterized by a higher degree of compatibility, functions as a template to facilitate uniform crystallization and effectively alleviates stress during the initial stages of crystallization. This, in turn, enhances the quality of the overlying perovskite film, prolongs the carrier lifetime, and optimizes the stress state. The 1D/3D PSCs fabricated using this interface design not only demonstrate high efficiency and stability but also exhibit excellent reproducibility, achieving a remarkable power conversion efficiency of 25.03% under standard AM 1.5 G one-sun illumination. After aging in an ambient air environment with a relative humidity of 55% for 1400 h, 94% of the initial efficiency is maintained for 1D/3D PSC.

Spiro-OMeTAD is the primary hole transport material (HTM) for high-efficiency and stable flexible perovskite solar cells (FPSCs). However, the slow oxidation rate and susceptibility to film cracking under stress in Spiro-OMeTAD lead to reduced device stability and efficiency. In this paper, a multi-functional novel self-healing nitroxide radical monomer, 4-[[5-(1,2-dithiolane-3-yl)-1-oxopentyl]amino]-2,2,6,6-tetramethylpiperidin-1-oxyl (DT-TEMPO), has been introduced to address these challenges. DT-TEMPO, on one side, enhances the hole mobility and conductivity by p-doping Spiro-OMeTAD, while boosting the charge transfer process from perovskite to Spiro-OMeTAD with an optimized energy level alignment on the other side. Additionally, DT-TEMPO endows a self-healing capability to Spiro-OMeTAD through the introduction of dynamic breaking and reconstructing disulfide bond. The optimized perovskite solar cells achieve impressive power conversion efficiencies, 25.69% on rigid substrates (certified 25.30%), 21.23% on rigid mini-modules, and 24.19% on flexible substrates. Remarkably, the FPSCs with DT-TEMPO retain over 90% of their initial efficiency even after 20 000 bending cycles (r = 6 mm) and recover to ≈95% of their initial value through the self-healing process.

Organic photodetectors (OPDs) are considered promising candidates for next-generation optoelectronic applications due to their mechanical flexibility, solution processability, and compatibility with large-area fabrication. Among them, near-infrared organic photodetectors (NIR-OPDs) have gained particular interest for use in biomedical monitoring, health diagnostics, and optical communication. However, their practical development is hindered by several critical challenges, including high dark current density, limited external quantum efficiency, and insufficient long-term stability. These issues are closely associated with interfacial defects, poor energy level alignment, and inefficient charge transport. In this review, we first examine the fundamental mechanisms behind dark current generation, with particular emphasis on the role of interfacial charge dynamics. We then critically summarize recent developments in interface materials and engineering strategies, covering both broadband and narrowband NIR-OPDs. Finally, we discuss the limitations of current strategies and propose future directions for interface engineering. This review aims to provide not only a comprehensive overview of the field but also mechanistic insights and forward-looking perspectives that can inspire further advancements in highperformance NIR-OPDs.