Achieving uniform crystallization across both top and buried interfaces in perovskite films is crucial for unlocking their full photovoltaic potential, yet remains an unresolved challenge. The buried interface, in particular, suffers from poor crystallization relative to the top surface, resulting in suboptimal crystal quality and increased defect densities. Here we propose a one-step strategy to induce the spontaneous formation of near-phase-pure two-dimensional perovskites at the buried interface via the introduction of organic cation halide salts in the perovskite precursor solution. Single-crystal structure analysis highlights the pivotal role of molecular engineering in facilitating the spontaneous formation of buried two-dimensional perovskite phases. The low dipole moments and planar rigidity structures of organic spacers promote their aggregation at perovskite grain boundaries, followed by their migration to the film's bottom interface. The two-dimensional perovskite layer simultaneously promotes uniform crystallization and efficient defect passivation at the buried interface, leading to a power conversion efficiency of 26.31% (certified 26.02%). Unencapsulated devices retain 95% of their initial power conversion efficiency after 1,000 hours of continuous illumination.

The photoactive alpha-phase perovskite plays a pivotal role in determining the efficiency and stability of perovskite solar cells (PSCs). Herein, we propose an innovative strategy for seed-assisted epitaxial growth based on latticematching. The pre-synthesized (GABA)2PbI4 single crystals as seeds are introduced into the three-dimensional (3D) perovskite precursor solution, successfully achieved the preferential and rapid formation of the photoactive alpha-phase at room temperature. In situ grazing-incidence wide-angle X-ray scattering (GIWAXS) reveals the seed-induced accelerated crystallization process of the alpha-phase perovskite. The highly matched lattice constants between the seeds and alpha-FAPbI3, the reduced nucleation barrier, and the suppressed delta-phase are analyzed to be the primary factors, ultimately resulting in the formation of vertically oriented, gradient-distributed perovskite films. Finally, FACs-based perovskite devices fabricated by using this method achieved a high efficiency of 24.15% and excellent stability, retaining over 90% of their initial efficiency after 900 h.

Ruddlesden-Popper perovskites are promising photovoltaic materials because their enhanced structural and environmental stability relative to their three-dimensional counterparts. However, weak interactions between organic spacer and the adjacent inorganic framework often undermine structural stability and impede charge transport. Here, we demonstrate that the hydrazide-based spacer, thiophene-2-hydrazide (ThCH), unexpectedly induces strong interlayer orbital coupling in 2D RP perovskites despite its monocyclic aromatic structure. It is found that the hydrazide group extends electronic conjugation and promotes orbital hybridization between ThCH and the adjacent inorganic framework, a phenomenon not observed in conventional single-ring aromatic spacers. This effect is further verified by benzo hydrazide, which shares a similar structural motif. Beyond promoting electronic coupling, the hydrazide functionality enhances film formation, yielding enhanced crystallization uniformity and facilitating efficient charge transport. Consequently, ThCH-based RP perovskite (nominal n = 4) devices achieve record efficiencies of 22.41% (certified 21.74%, 0.074 cm2) for small-area devices and 20.74% (certified 20.01%, 1.015 cm2) for large-area devices, the highest reported for quasi-2D RP PSCs. This study establishes a molecular design strategy that uses multifunctional hydrazide modules to overcome the electronic insulation of single-ring aromatic spacers, enabling robust and efficient RP PSCs.

This work highlights the latest advances in the fast growth of high-quality perovskite single crystals in solutions and sets forth the relative methodologies, mechanisms, challenges and perspectives.

Polyvinylidene fluoride (PVDF) based polymer solid electrolytes are crucial plastic components in all-solid-state lithium-ion batteries (ASLIBs). However, the large-scale application of PVDF-based solid electrolytes without proper treatment will cause persistent environmental contamination and resource waste, thus highlighting an urgent need for effective recovery strategies. Herein, we firstly propose a hydrogen bond-driven strategy with ultrasonic assistance for ultrafast and eco-friendly recovery of PVDF nanoplastic from polymer solid electrolytes of ASLIBs. Utilizing the proposed hydrogen bond-driven strategy, a maximum F leaching efficiency of 98.2% from PVDF nanoplastic can be attained within a short timeframe and under mild conditions using eco-friendly solvents. Compared with traditional methods, ultrasonic treatment exhibits a significantly improved leaching efficiency of approximately 88%. This ultrafast recovery and notable enhancement can be attributed to the breakdown of C-F bonds in PVDF, which is realized by regulating hydrogen bond networks in green solvents combined with ultrasonic treatment. This study presents a novel strategy for the green, rapid and significantly enhanced recovery of PVDF nanoplastic from spent polymer solid electrolytes of ASLIBs.

Photolithographic patterning of perovskite nanocrystals (PeNCs) is pivotal for realizing color-conversion schemes in full-color Micro-LED displays; however, this process is currently hindered by severe material degradation and a pervasive reliance on toxic organic solvents. Herein, we propose a robust PeNC photoresist strategy designed for compatibility with eco-friendly green solvents, specifically enabling the use of benign ethanol as a developer for high-resolution patterning. By synthesizing PeNCs directly within isobornyl acrylate (IBOA) monomers and engineering an in situ SiO2 encapsulation layer via hydrolysis, we achieve superior material stability. Remarkably, the resulting PeNC@SiO2/IBOA composites retain bright fluorescence after 3480 h of ethanol immersion, whereas uncoated controls quench completely within 96 h. Leveraging this stability, we successfully patterned color conversion pixels with dimensions of 20 µm × 10 µm via photolithography with green solvent ethanol as the developer, which retain 80.3% of their initial photoluminescence quantum yield (PLQY) post-lithography. The successful fabrication of highly uniform red, green, and blue (RGB) pixel arrays demonstrates the significant potential of this green, high-performance lithography strategy of PeNCs for next-generation Micro-LED displays.

Sustainable recycling of lithium-ion battery (LIB) cathodes is essential for mitigating resource depletion and environmental pollution. However, the inherent trade-off between selectivity and efficiency remains a critical barrier limiting the performance of current recycling technologies. Herein, we demonstrate that the selectivity and efficiency of metal leaching from LiCoO2 cathodes in spent LIBs can be effectively mediated by the hydrogen bond donor (HBD) in sustainable low-melting mixture solvents. Employing phosphorous acid as the HBD in a betaine:phosphorous acid-based solvent system yields ultrahigh Li/Co selectivity during leaching from the LCO cathode. In contrast, high overall recovery efficiencies for both Li and Co are achieved when phosphoric acid serves as the HBD in a betaine:phosphoric acid-based solvent system.

Perovskite single crystals (PSCs) are highly promising direct X-ray detection materials, whereas the mechanical brittleness and thermal instability easily bring about stress cracking and structural decomposition under a conventional bonding process, hindering integrated applications. In this work, we developed a photopolymerization-induced heterogeneous bonding technology based on 4-acryloylmorpholine (ACMO) for monolithic PSC integration, which enables effective bonding within seconds via a liquid film transfer method. The interfacial coordination effect between ACMO and PSCs simultaneously achieves defect passivation for the buried surface of PSCs and robust mechanical bonding with tensile and shear strengths of up to 1.81 and 1.50 MPa, respectively. Furthermore, polymerized ACMO has a high resistivity of 7.72 × 1012 Ω·cm that effectively suppresses dark current in the integrated devices. Compared with the control crystal, the dark current of the integrated device is reduced by 2 orders of magnitude, while the limit of detection (LOD) for X-ray detection improves 20-fold. The 5.6% relative standard deviation of dark currents among 6 × 6 pixels and 96% performance retention after 30 days of storage confirm the reliable uniformity and stability. This work provides a novel technical solution for the heterogeneous bonding of PSCs, facilitating the further development of high-performance PSC-integrated optoelectronic devices.

Photocatalysis offers a promising solution to global energy and environmental challenges. Combing pollution degradation reaction with the water-splitting hydrogen production system is of great significant to take full use of electrons and holes, but it faces challenges in the exploration of catalysts with high performance and clear reaction pathways. In this work, we reported a CdS/MoS2/MnO2 (CdSx/Mo/Mny) ternary hybrid with clearly defined spatial position by introducing MoS2 and MnO2 on CdS nanorods through the combination of chemical occupying strategy with the photo-deposition method. When reacted in a TC solution with the absence of cocatalyst nor sacrificial agent, a hydrogen evolution rate of 1.06 mmol/g/h coupled with simultaneous 96.8% degradation of TC can be reached on the optimized CdS1/Mo/Mn45 composite. The formation of spatially isolated yet uniformly distributed reaction centers contributes most to the realization of high performance dual functional photocatalytic reaction, which providing dedicated regions for redox processes while optimizing inter-site distance to minimize charge recombination. This study presents a novel strategy for designing highly active dual-function photocatalysts capable of efficient simultaneous oxidation and reduction reactions, demonstrating great potential for synergistic energy and environmental applications.

Fullerene-based materials, particularly [6,6]- phenyl-C61-butyric acid methyl ester (PC61BM), are extensively employed as electron transport materials (ETMs) in inverted perovskite solar cells (PSCs) due to their superior electron transport properties. However, their insufficient passivation capability and tendency to aggregate in films can lead to interfacial charge accumulation and charge carrier recombination losses, ultimately compromising both the efficiency and stability of PSCs. To address these challenges, we developed a novel fullerene derivative, PC61BP, by grafting a cyano-phosphate (CNPhP) functional group to fullerene. The phosphate moiety and-CN group in PC61BP can coordinate with undercoordinated Pb2+ ions on the perovskite surface, facilitating defect passivation and suppressing charge nonradiative recombination. Importantly, the incorporation of the CNPhP group can modulate intermolecular interactions among PC61BP molecules, preventing aggregation and promoting the formation of a more uniform film. Consequently, the inverted devices using PC61BP as the ETM achieve a champion power conversion efficiency (PCE) of 26.01%, markedly outperforming the PC61BM-based control device (PCE = 24.59%), along with improved stability. Moreover, the 1.01 cm2 devices using PC61BP as the ETM achieve a high efficiency of 24.48%. This study offers a promising strategy for advancing the performance of inverted PSCs through the rational design of fullerene-based ETMs.

Charge transport is an important property that influences the stability of organic solar cells (OSCs). While decreased average charge mobility during degradation is recognized as an essential factor reducing device stability, the dispersion property of charge transport is often overlooked. The dispersion parameter characterizes the dispersion of transit times in charge transport. A high dispersion parameter typically indicates a significant population of slow charge carriers in OSCs, which could introduce more charge recombination and ultimately compromise device stability. In this work, we demonstrate that the combined effect of dispersion parameter and charge mobility serves as a key indicator of degradation pathways, underscoring the critical role of the initial morphology of the active layer in device stability. This work not only establishes a morphology-transport stability framework for enhancing the charge transport stability but also discovers the significance of sustaining a balanced mobility-dispersion property for ensuring the long-term stability of OSCs.

All-perovskite tandem solar cells (AP-TSCs) offer the potential to surpass the Shockley-Queisser (S-Q) limit of single-junction perovskite solar cells (PSCs). Nevertheless, the wide-bandgap (WBG) sub-cells suffer from severe open-circuit voltage (V OC) losses induced by surface defects and energy-level mismatch at the WBG perovskite/C60 interface. Herein, we implemented a bimolecular passivation strategy by achieving hetero-spatial distribution of piperazinium bromide (PipBr) and 3-(methylthio) propylamine hydrobromide (3MTPABr) in the WBG perovskite surface layer. Pip+ facilitates a reconstruction of the perovskite surface to form an anchored-gradient passivation region, while 3MTPA+ constructs an ultrathin low-dimensional perovskite capping layer atop this reconstructed region. This thumbtack-type spatial distribution of the two molecules effectively passivates surface defects and optimizes the energy-level alignment at the perovskite/C60 interface, achieving suppressed interfacial non-radiative recombination, enhanced charge transport, and improved surface hydrophobicity. Consequently, single-junction gas-quenched MA-free WBG (similar to 1.76 eV) PSCs achieve a power conversion efficiency (PCE) of 20.80% (with a certified value of 20.02%) and retain 91.1% of their initial PCE after 600 h of operation under 1.0 sun illumination, demonstrating the importance of spatial molecular distribution in WBG perovskite co-passivation. Notably, the fabricated 2-terminal AP-TSC device attains a PCE of 28.34%, highlighting its considerable potential for AP-TSC applications.

Developing low-cost active layer systems that offer both high performance and non-halogenated solvent processing is a critical step towards the commercialization of organic solar cells (OSCs). Herein, we design and synthesize a fully non-fused ring electron acceptor (NFREA), DTBM22, with a material-only cost of 12.0 $ g-1 and well-ordered molecular stacking. The non-halogenated solvent processed DTBM22-based OSCs achieve a PCE of 13.5%. Interestingly, DTBM22 forms an alloy-like phase when blended with the low-cost fully NFREA DTB22. Compared to pristine DTB22 films, the blend improves the exciton diffusion length from 25.7 to 30.2 nm and reduces the exciton dissociation energy barrier from 10.4 to 6.7 meV. When OSCs are fabricated using a non-halogenated solvent, the control DTB22-based OSC delivers a good PCE of 16.9%, while the DTBM22:DTB22-based OSC achieves an outstanding PCE of 18.0%, which is the highest PCE value reported to date for both NFREA-based and fully NFREA-based OSCs processed using non-halogenated solvents. This study offers a new insight into developing high-performance, low-cost, non-halogenated solvent-processed OSCs.

Stretchable organic solar cells (OSCs) hold significant promise as light-harvesting power sources in wearable electronics. Physical blending highly-deformable elastomer into rigid photovoltaic components represents a simple and effective approach to enhance film stretchability. However, the mechanical and photovoltaic performance of elastomer-based active layers are generally inferior to those achieved through chemical approaches. Herein, we report a high-performance stretchable active layer that combines photo crosslinking with sequential deposition of an elastomer-based ternary system poly[2,6-(4,8-bis(5-(2-ethylhexyl-3-fluoro)thiophen-2-yl)-benzo[1,2-b:4,5-b']dithiophene))-alt-5,5'-(5,8-bis(4-(2-butyloctyl)thiophen-2-yl)dithieno[3',2':3,4;2'',3'':5,6]benzo[1,2-c][1,2,5]thiadiazole)] (D18)/2,2'-((2Z,2'Z)-((12,13-bis(2-ethylhexyl)-3,9-diundecyl-12,13-dihydro-[1,2,5]thiadiazolo[3,4-e]thieno[2'',3'':4',5']thieno[2',3':4,5]pyrrolo[3,2-g]thieno[2',3':4,5]thieno[3,2-b]indole-2,10-diyl)bis(methanylylidene)bis(5,6-difluoro-3-oxo-2,3-dihydro-1H-indene-2,1-diylidene))dimalonitrile) (Y6): polystyrene-block-poly(ethylene-ran-butylene)-block-polystyrene (SEBS), achieving a power conversion efficiency of 15.38% and a crack-onset strain of 35.91%. Crosslinking D18 with an azide compound ethane-1,2-diyl bis(4-azido-2,3,5,6-tetrafluorobenzoate) (2BX) in the bottom layer not only produces a 3D covalent network, but also results in a low-crystallinity film with a reduced glass transition temperature. These structure changes contribute to delayed large-scale chain slippage and enhanced strain energy dissipation, leading to approximately 100% and 40% improvements in the stretchability of D18 film and full active layer. Moreover, the charge generation and transport behaviors are just slightly affected with moderate microstructure change, enabling the device to retain 94% of initial efficiency. Ultimately, the optimal active layer achieves an efficiency-stretchability factor of 5.52%, ranking among the highest reported values for stretchable active layer systems.

Because of the susceptibility of perovskite single crystals (PerSCs) to moisture- and oxygen-induced degradation, the simultaneous improvement of their environmental durability and optoelectronic properties remains an intractable challenge. Herein, we develop an in situ encapsulation approach for PerSCs using a polymerizable ionic liquid, named 1-vinyl-3-butylimidazolium bis(trifluoromethylsulfonyl)imide (Bvim-TFSI), as an additive. Bvim-TFSI addition can facilitate the thermokinetic growth process and eliminate the need for intricate post-treatments owing to its self-cleaning property. More importantly, the in situ radical polymerization of Bvim-TFSI on the crystal surface leads to the formation of an oligomeric encapsulation layer, imparting an enhanced environmental robustness to the as-fabricated PerSC, with no observable degradation after 10 months of air exposure. The resulting MAPbI3 single crystal exhibits an X-ray detection sensitivity of 1.80 & times; 105 mu C Gyair -1 cm-2 with a low limit of detection of 10.37 nGyair s-1. Moreover, the PerSC-based device demonstrates nearly 100% performance retention after 30 days of storage in ambient air without additional protection. This study provides a facile route for the fabrication of high-quality and durable PerSCs toward optoelectronic applications.

Chiral hybrid perovskites exhibit great potential in chiral optoelectronics, but suffer from insufficient intrinsic chirality due to inefficient chirality induction from the organic cation. Here, we unravel that extending the conjugation length of organic cation enhances the intrinsic chirality of 1D chiral hybrid perovskite single crystals (CHPSCs). The extended conjugation length of organic cation intensifies the inorganic-framework torsion and regulates the band-edge configuration through improved hydrogen bonding and pi-electron interactions, thereby strengthening intrinsic crystalline chirality. Benefiting from the superior intrinsic chirality and intensified intermolecular interaction, the 1-(1-naphthyl)ethylammonium (NEA) based 1D CHPSC achieves a high circularly polarized photocurrent anisotropy factor of 0.38 with a specific detectivity of 1.03 & times; 1011 Jones. Furthermore, it is experimentally found that the 1D CHPSC inherits the same structural asymmetry from its corresponding chiral ligand, enabling actual chirality transfer. This study provides deeper insight into advancing the intrinsic chirality of CHPSCs for high-performance optoelectronic applications.

The advancement of intrinsically stretchable photovoltaic films is essential for powering next-generation wearable electronics through all-polymer solar cells (APSCs). While blending with elastomeric materials has emerged as an effective strategy to enhance mechanical robustness, the fundamental microstructural evolution under strain remains poorly understood. Here we introduce and implement a synchrotron-based in situ stretching X-ray scattering technique to directly probe nanoscale morphological changes in real time. Incorporating a styrene-isoprene-styrene elastomer SIS induces enhanced π-π stacking intensity both parallel and perpendicular to the stretching direction. The resulting stretchable APSCs achieve a record-high efficiency over 16% and exceptional mechanical stability, retaining over 80% of initial efficiency at 60% strain and 81% after 1000 stretching cycles at 40% strain. Furthermore, power output remains stable under strains of up to 60%, and the mechancial parameters are well predicted by the Coral-Patel model. This study provides critical insights for elastomer selection and microstructure design in stretchable electronics.

The regulation strategy to tune the recovery of cathode from sodium-ion batteries (SIBs) is of great significance. However, traditional strategies involving temperature, duration, and additives often lead to high energy demands, time deficiencies, notable environmental pollution, or complicated separation processes. Here, we propose a sustainable strategy based on the synergistic regulation of basicity and hydrophobicity to regulate the cathode recycling from SIBs using amino acid-based deep eutectic solvents (DESs) with low energy consumption, high time efficiency and simple process. The metal leaching efficiency from SIBs cathode could be tuned by dual-regulation of high basicity and moderate hydrophobicity. The basicity of amino acid-based DESs shows a weak positive correlation with the metal leaching efficiency, while hydrophobicity of amino acid exhibits a trend of initially increasing and then decreasing with metal leaching efficiency. After reasonable tunability of basicity and hydrophobicity, DESs glycine:lactic acid (1:12) is capable of recycling 87.5% Na and 83.3% Fe from the sodium iron phosphate cathode of SIBs at a mild temperature of 80°C for 24 h with a liquid-to-solid ratio of 50:1.

Conventional methods for recycling metals from the leachate of spent sodium-ion batteries (SIBs) cathodes encounter several challenges, such as high energy consumption, complicated process and environmental pollution. Herein, a capric acid-driven three-phase antisolvent precipitation (CTAP) strategy is used for the low-energy and sustainable recovery of metal and lixiviant from the leachate associated with SIBs cathode vanadium phosphate sodium (NVP) and low-melting mixture solvents (LoMMSs). The CTAP strategy results in a three-phase precipitation, with the upper layer representing the capric acid phase, the middle layer consisting of the lixiviant phase, and the bottom layer comprising the solid phase. Through the CTAP strategy, capric acid achieves the antisolvent precipitation efficiencies of 86.8% for Na and 50.5% for V when applied to leachate from NVP and LoMMS polyethylene glycol 200:phytic acid; nevertheless, capric acid is ineffective in precipitating metals from leachate derived from LoMMSs that combine polyethylene glycol 200 with citric acid, benzoic acid, urea, or acetamide. Additionally, the LoMMSs using polyethylene glycol 200:phytic acid as the lixiviant achieve maximum leaching efficiencies of 99.1% for Na and 94.4% for V from NVP at a mild temperature of 80 °C over 24 hours, with a liquid-to-solid ratio of 200 after optimizing factors, such as hydrogen bond donors, molar ratios, temperature, time, liquid-to-solid ratio and scalability. This work provides an energy-saving, process-simplified and eco-friendly strategy for the separation of metals from SIBs leachate.

Chitosan, as one of the most sustainable biomaterials in green and renewable resources, has been widely practised because of its good biocompatibility and biodegradability. However, the challenge of limited solubility of chitosan in neutral or alkaline media (pH >= 6.5) has been clearly pinpointed. In this study, a novel water-soluble and fiber-reactive O-[(2-hydroxy-3-trimethylammonium)propyl] chloride oxidized chitosan (O-HACOC) was prepared with a view to developing the antibacterial finishing agent of textile fibers. The resulted O-HACOC contained dicationic groups of quaternary ammonium salt groups at C6 site and amino groups at C2 position in chitosan backbone, which offered good water solubility and antibacterial activity in the wider pH ranges. The water solubility of O-HACOC prepared under the optimized process can reach 23.7 g/100 mL, and its minimum inhibitory concentrations were lower than 0.0625 mg/mL against Escherichia coli and 0.125 mg/mL against Staphylococcus aureus, respectively. Meanwhile, O-HACOC also showed the high antioxygenic property. This work provides ideas for the design and development of novel functional chitosan derivatives.