http://onlinelibrary.wiley.com/rss/journal/10.1002/(ISSN)1521-4095

Disorder in a crystal is rarely randomly distributed but instead can involve extra chemical order. This could offer a new degree of freedom that is essential to designing materials with emergent properties. This research achieves the continuous regulation of vacancy order from long-range order to short-range order in cation-deficient half-Heusler crystals. Engagingly, various functionalities present significant changes accompanying the evolution of vacancy order.

Extra chemical order within periodic crystalline lattices offers a promising approach for designing materials with emergent functionalities. However, achieving tunable extra chemical order in crystalline materials remains challenging. Here, it is found that the vacancy order in cation-deficient half-Heusler crystals V1- δ CoSb can be tuned from long-range order (LRO) to short-range order (SRO), or vice versa. The vacancy LRO and SRO configurations are uncovered by scanning transmission electron microscopy analysis and Monte Carlo simulations. Remarkably, the evolution of vacancy order induces profound changes in electrical, magnetic, and thermal properties, as well as hydrogen storage characteristics. In particular, the electronic density of state effective mass exhibits a nearly threefold increase, while ferromagnetism emerges from infancy when tuning the vacancy order from LRO to SRO. These results elucidate the local chemical order-property relationship and highlight the great potential of achieving desirable functionalities by designing extra chemical order in crystalline solids.

High-efficiency narrowband emissive themally activated delayed flurescence (TADF) polymers are realized by incorporating silicon─carbon σ-bond saturated spacers between multiresonance TADF units and polycarbazole backbone. The polymers exhibit a high photoluminescence quantum yield of 97% and external quantum efficiency of up to 30.2% with a narrow full width at half maximum of 42 nm in organic light-emitting diodes.

Achieving both high-efficiency and narrowband emission in thermally activated delayed fluorescence (TADF) polymers remains a formidable challenge. In this work, a proof of concept for narrowband-emissive TADF polymers with a partially conjugated structure is proposed by embedding a silicon─carbon σ-bond saturated spacer between the multiresonance (MR) TADF unit and the polycarbazole backbone. A series of TADF polymers PSix (x = 1, 3, and 6) is then prepared and characterized. All the polymers show narrowband emission with full width at half maximum (FWHM) values of 28–30 nm in a toluene solution. Impressively, polymer PSi3 has the highest photoluminescence quantum yield, reaching 97%, in the doped films due to the efficient reverse intersystem crossing process. The solution-processed devices based on PSi3 exhibit the best performance with a maximum external quantum efficiency (EQE max) of 28.8% and an FWHM of 42 nm. By employing the TADF molecule 5Cz-TRZ as the sensitizer, enhanced device performance with an EQE max of 30.2% is achieved, which is in the first tier among the MR-TADF polymers reported to date. This work provides an effective strategy for achieving highly efficient and narrowband-emissive TADF polymers by controlling the σ-bond saturated spacer between the MR-TADF chromophore and the polymer backbone.

A noninvasive second near-infrared long-wavelength nanosensor (C8R-DSNP) for real-time monitoring of immune cell-tumor interactions in vivo is reported. The sensor detects caspase-8 activation during natural killer cells-induced apoptosis in tumor cells, providing dynamic, early-stage imaging within 4.5 h of treatment. This approach offers valuable insights for optimizing immunocytotherapy strategies with rapid, in vivo feedback.

Immunocytotherapy holds significant promise as a novel cancer treatment, but its effectiveness is often hindered by delayed responses, requiring evaluations every 2–3 weeks based on current diagnostic methods. Early assessment of immune cell-tumor cell interactions could provide more timely insights into therapeutic efficacy, enabling adjustments to treatment plans. In this study, a noninvasive nanosensor (C8R-DSNP) for real-time monitoring of in vivo immune cell activities in the second near-infrared long-wavelength (NIR-II-L) window (1500–1900 nm), which offers deep tissue transparency, is reported. The C8R-DSNP responds rapidly to caspase-8, a key apoptotic signaling molecule generated during interactions between natural killer (NK-92) cells and tumor cells. Using ratiometric NIR-II-L fluorescence imaging, dynamic in vivo observations of NK-92 cells' engagement with tumor cells in a mouse model are captured. These results demonstrate tumor cells apoptosis that happens as early as 4.5 h after NK-92 cells infusion. Additionally, in vitro urine imaging confirmed the initiation of apoptosis via cleaved fluorescent small molecules, while single-cell tracking within blood vessels and tumors further elucidated immune cell dynamics. This real-time NIR-II-L monitoring approach offers valuable insights for optimizing immunocytotherapy strategies.

This study presents a novel composite solid-state polymer electrolyte incorporated dielectric BaTiO3 nanofillers (PDB) for advanced high-voltage all-solid-state lithium batteries. The design achieves a tailored coordination structure, diminished space charge layer, improved ion transport, and enhanced oxidative stability, making this approach a promising strategy for practical long-cycling all-solid-state lithium batteries.

The poor structural stability of polymer electrolytes and sluggish ion transport kinetics of interfaces with cathode limit the fundamental performance improvements of polymer all-solid-state lithium metal batteries under high voltages. Herein, it is revealed that by introducing dielectric BaTiO3 in an in-situ polymerized composite solid-state electrolyte, the generated interaction between the ether group of polymer electrolyte and dielectric material could effectively regulate the lithium-ion (Li+) coordination structure to achieve an oxidative potential higher than 5.2 V. The dielectric BaTiO3 with spontaneous polarization also weakens the space charge layer effect between the cathode and electrolyte, facilitating fast Li+ transport kinetics across the cathode/electrolyte interfaces. The all-solid-state LiNi0.8Co0.1Mn0.1O2/Li batteries with the dielectric composite solid-state electrolyte exhibit an ultra-long cycling life of 1800 and 1300 cycles at room temperature under high cut-off voltages of 4.6 and 4.7 V, respectively. This work highlights the critical role of dielectric materials in high-performance solid-state electrolytes and provides a promising strategy to realize high-voltage long-life all-solid-state lithium metal batteries.

A Li plating regulation strategy that transforms dead Li plating into reversible active Li plating is proposed by using a lithium dendrite inhibitor to realize safe and long-lifespan LIBs. Remarkably, only 1 wt.% single-atom manganese (SAMn) in the Gr anode (Gr-SAMn) is sufficient to achieve a significant improvement, and the amount of dead Li on the Gr anode can be reduced by 90%.

Under harsh conditions, such as high-rate and low-temperature charging, part of Li ions cannot intercalate into the graphite (Gr) particles and will form dendrite-like Li plating, causing capacity fading and serious safety hazards in commercial lithium-ion batteries (LIBs). Herein, instead of eliminating the Li plating, a Li plating regulation strategy that transforms dead Li plating into reversible active Li plating is proposed by using a lithium dendrite inhibitor to realize safe and long-lifespan LIBs. Remarkably, only 1 wt.% single-atom manganese (SAMn) in the Gr anode (Gr-SAMn) is sufficient to achieve a significant improvement, thus both the volumetric and mass-energy density remain roughly unaffected. The amount of dead Li on the Gr anode can be reduced by 90%, thereby enabling much-improved pouch cell performance at high rates and low temperatures. The capacity retention of the Gr-SAMn||NCM811 pouch cell is 86.2% (23.0% higher than that of the pristine Gr||NCM811 pouch) for 1500 cycles at 2 C, and the cell can even be cycled at 5C charge. Even cycling at −20 °C, the average coulombic efficiency (CE) can be improved from 97.95% to 99.94% by using SAMn additive. Hence, this promising strategy provides a novel alternative to solve the Li plating issue.

The carrier transport behavior is regulated rather than the previously oversimplified limitation strategy to reduce losses and enhance energy storage efficiency. It is expected to offer a novel and effective theoretical basis for the design and fabrication of advanced polymer dielectrics with high capacitive energy storage level at harsh environments.

Polymer dielectrics with high capacitive energy-storage levels in harsh environments have become key components in electrostatic capacitors. However, excessive losses in polymer dielectrics caused by high carrier densities at high temperatures and strong electric fields often result in low energy storage efficiency, which is the most challenging problem that urgently needs to be solved. In existing studies, the losses are mainly suppressed by limiting carrier formation; however, it is very challenging to completely limit carrier formation, especially at high temperatures and strong electric fields. Therefore, this perspective proposes to regulate the carrier transport behavior through “guiding/constraining/blocking” forms rather than the previously oversimplified carrier limitation strategy, which further clarifies dominant structure factors that inhibit carrier transport to reduce losses and enhance energy storage efficiency. Meanwhile, the influence of different structural designs on carrier transport behavior, individually or collaboratively, must be systematically studied to determine the specific mode of carrier transport behavior, thereby establishing a relationship between carrier transport behavior and energy storage efficiency. The presented perspective is expected to offer a novel and effective theoretical basis for the design and fabrication of advanced polymer dielectrics with high capacitive energy storage levels in harsh environments.

The degradable additive couple is developed to enable pure and preferential-oriented α-FAPbI3 perovskite with a bandgap of 1.489 eV and robustness against light, heat, and moisture over 1000 h, without the additive residue. The resultant perovskite solar cells achieve a power conversion efficiency of 25.20% with a short current density of 26.40 mA cm−2 and long-term operational stability of over 1000 h.

Pure black-phase FAPbI3 has always been pursued because of its ideal bandgap (E g) and high thermal stability. Here, a pair of sacrificial agents containing diethylamine hydrochloride (DEACl) and formamide (Fo) is reported, which can induce the oriented growth of black-phase FAPbI3 along (111) and will disappear by the aminolysis reaction during perovskite annealing, retaining the E g of FAPbI3 as 1.49 eV. In addition, the tensile strain of the target FAPbI3 is found to be mitigated with a stabilized black phase due to the tilt of FA+. The devices based on the pure and stable black-phase (111)-FAPbI3 achieved a power conversion efficiency of 25.2% and 24.2% (certified 23.51%) with an aperture area of 0.09 and 1.04 cm2, respectively. After 1080 h of operation at the maximum power point under 1-sun illumination (100 mW cm−2), the devices maintained 91.68 ± 0.72% of the initial efficiencies.

A versatile assembly method is developed to uniformly assemble 2D single-crystal copper nanosheets (Cu NS) onto substrates with complex shapes via ultrasonication process. This technique leverages cavitation effects to deposit monolayer Cu NS films with minimal overlap. The assembly is optimized by tuning solvent polarity and substrate surface energy. Demonstrated applications include a resistive heater, highlighting the potential in flexible electronics.

Scalable and cost-effective fabrication of conductive films on substrates with complex geometries is crucial for industrial applications in electronics. Herein, an ultrasonic-driven omni-directional and selective assembly technique is introduced for the uniform deposition of 2D single-crystalline copper nanosheets (Cu NS) onto various substrates. This method leverages cavitation-induced forces to propel Cu NS onto hydrophilic surfaces, enabling the formation of monolayer films with largely monolayer films with some degree of nanosheet overlap. The assembly process is influenced by solvent polarity, nanosheet concentration, and ultrasonic parameters, with non-polar solvents significantly enhancing Cu NS adsorption onto hydrophilic substrates. Furthermore, selective assembly is achieved by patterning hydrophobic and hydrophilic regions on the substrate, ensuring precise localization of Cu NS films. The practical potential of this approach is demonstrated by fabricating a Cu NS-coated capillary tube heater, which exhibits excellent heating performance at low operating voltages. This ultrasonic-driven and selective assembly method offers a scalable and versatile solution for producing conductive films with tailored geometries, unlocking new possibilities for applications in flexible electronics, energy storage, and wearable devices with complex structural requirements.

This study introduce a novel approach to enhancing cathode-SPE compatibility by utilizing the same poly(ionic liquid) (PolyIL)-based material in both the SPE and the cathode binder. A modified biomass-based PolyIL substrate, enriched with highly negatively charged C═O and ─OH groups, is incorporated into the SPE to improve Li+ migration and strengthen its mechanical properties. The Li||LiFePO₄ cell, assembled via in situ photopolymerization, demonstrate stable cycling for over 1100 cycles, while the Li||NCM811 cell operated reliably at a high cut-off voltage of 4.8 V for 100 cycles.

Lithium metal batteries (LMBs) with solid polymer electrolytes (SPEs) offer higher energy density and enhance safety compared to the Li-ion batteries that use a graphite anode and organic electrolytes. However, achieving long cycle life for LMBs while enabling the use of high-voltage cathodes required the compatibility between cathode-SPE, rather than focusing solely on the individual components. This study presente a dual-functional poly(ionic liquid) (PolyIL)-based material that simultaneously serves as an SPE matrix and a cathode binder, constructing a cathode-SPE interface with exceptional (electro)chemical compatibility owing to the high ionic conductivity and wide electrochemical stability window. Additionally, a modified cellulose acetate (CA)-based PolyIL substrate, enriched with C═O and ─OH groups, is designed rationally and incorporated to assist the Li+ migration, leveraging their highly negative charge, and enhancing the mechanical strength of the SPE. Furthermore, an in situ polymerization approach is employed to assemble the cells, improving the physical compatibility at the cathode-SPE interface. As a result, the Li||LFP cell demonstrate stable cycling beyond 1100 cycles, and the Li||NCM811 cell reliably operates at a high cut-off voltage of up to 4.8 V.

Synthesis of topological semimetal TaAs2 nanowires in situ encapsulated with a thin SiO2 shell unravel a richness of intertwined topological phases manifested by their magnetotransport features: A near-room-temperature metal-to-insulator transition, strong expressions of topologically nontrivial surface transport, giant magnetoresistance with direction-dependent sign reversal, chiral anomaly, and a unique double pattern of Aharonov–Bohm oscillations.

Nanowires (NWs) of topological materials are emerging as an exciting platform to probe and engineer new quantum phenomena that are hard to access in bulk phase. Their quasi-1D geometry and large surface-to-bulk ratio unlock new expressions of topology and highlight surface states. TaAs2, a compensated semimetal, is a topologically rich material harboring nodal-line, weak topological insulator (WTI), C2-protected topological crystalline insulator, and Zeeman field-induced Weyl semimetal phases. We report the synthesis of TaAs2 NWs in situ encapsulated in a dielectric SiO2 shell, which enable to probe rich magnetotransport phenomena, including metal-to-insulator transition and strong signatures of topologically nontrivial transport at remarkably high temperatures, direction-dependent giant positive, and negative magnetoresistance, and a double pattern of Aharonov–Bohm oscillations, demonstrating coherent surface transport consistent with the two Dirac cones of a WTI surface. The SiO2-encapsulated TaAs2 NWs show room-temperature conductivity up to 15 times higher than bulk TaAs2. The coexistence and susceptibility of topological phases to external stimuli have potential applications in spintronics and nanoscale quantum technology.

A thermo-electrochemically compatible polymer electrolyte is proposed with a locally conjugated structure through self-regulation of paired tertiary anilines coupled with in situ polymerization, which significantly reconstructs an improved Li+ solvation and enhances electrode/electrolyte interfacial stability of LMBs. This concept provides an important theoretical basis and technical means for achieving practical high energy/power density LMBs.

Pursuing high energy/power density lithium metal batteries (LMBs) with good safety and lifespan is essential for developing next-generation energy-storage devices. Nevertheless, the uncontrollable degradation of the electrolyte and the subsequent formation of inferior electrolyte/electrode interfaces present formidable challenges to this endeavor, especially when paring with transition metal oxide cathode. Herein, a fireproof polymeric matrix with a local conjugated structure is constructed by 4,4′-methylenebis (N, N-diglycidylaniline) (NDA) monomer via in situ polymerization, which promotes the use of ester-based liquid electrolyte for highly stable LMBs. The conjugated tertiary anilines in this PNDA electrolyte effectively tune the Li+ solvation sheath and generate conformal protective layers on the electrode surfaces, resulting in excellent compatibility with both high-voltage cathodes and Li-metal anodes. Moreover, the accumulated electron density endows PNDA with a powerful capability to seize and eliminate the corrosive hydrofluoric acid, which strikingly mitigates the irreversible structure transformation of LiNi0.8Mn0.1Co0.1O2 (NMC) particles. As a result, the PNDA-based Li||LiFePO4 and Li||NMC cells reach excellent electrochemical and safety performance. This study provides a promising strategy for the macromolecular design of electrolytes and emphasizes the importance of “local conjugation” within the polymers for LMBs.

An efficient and safe circular-RNA delivery system circSCMH1@LNP1 is developed for direct nose-to-brain delivery of circRNA SCMH1 to ischemic lesions. Experiments demonstrate that intranasally administrated circSCMH1@LNP1 significantly accumulates in the peri-infarct region of PT stroke mice, thereby improving functional recovery by enhancing synaptic plasticity, vascular repair, neuroinflammation relief, and myelin sheath formation.

Ischemic stroke represents one of the leading cerebrovascular diseases with a high rate of mortality and disability globally. To date, there are no effective clinical drugs available to improve long-term outcomes for post-stroke patients. A novel nucleic acid agent circSCMH1 which can promote sensorimotor function recovery in rodent and nonhuman primate animal stroke models has been found. However, there are still delivery challenges to overcome for its clinical implementation. Besides, its effects on post-stroke cognitive functions remain unexplored. Herein, lipid nanoparticle circSCMH1@LNP1 is established to deliver circSCMH1 and explore its therapeutic efficacy comprehensively. Distribution experiments demonstrate that intranasal administration of circSCMH1@LNP1 significantly increases circSCMH1 distribution in the peri-infarct region and reduces its non-specific accumulation in other organs compared to intravenous injection. Therapeutic results indicate that circSCMH1@LNP1 promotes synaptic plasticity, vascular repair, neuroinflammation relief, and myelin sheath formation, thereby achieving enhanced sensorimotor and cognitive function recovery in post-stroke mice. In conclusion, this research presents a simple and effective LNP system for efficient delivery of circSCMH1 via intranasal administration to repair post-stroke brain injury. It is envisioned that this study may bridge a crucial gap between basic research and translational application, paving the way for clinical implementation of novel circSCMH1 in post-stroke patient management.

Super-hard wood-based composites (WBC) are designed and developed inspired by the mesoscale homogeneous lignification process intrinsic to tree growth. This innovative hybrid structure is achieved by leveraging the infusion of low-molecular-weight phenol formaldehyde resin into the cell walls of thin wood slices, followed by a unique multi-layer construction and high-temperature compression.

The growing demand for high-strength, durable materials capable of enduring extreme environments presents a significant challenge, particularly in balancing performance with sustainability. Conventional materials such as alloys and ceramics are nonrenewable, expensive, and require energy-intensive production processes. Here, super-hard wood-based composites (WBC) inspired by the meso-scale homogeneous lignification process intrinsic to tree growth are designed and developed. This hybrid structure is achieved innovatively by leveraging the infusion of low-molecular-weight phenol formaldehyde resin into the cell walls of thin wood slices, followed by a unique multi-layer construction and high-temperature compression. The resulting composite exhibits remarkable properties, including a Janka hardness of 24 382 N and a Brinell hardness of 40.7 HB, along with exceptional antipiercing performance. The created super-hard, sustainable materials address the limitations of nonrenewable resources while providing enhanced protection, structural stability, and exceptional resilience. The WBC approach aligns with UN Sustainable Development Goals (SDGs) by offering extra values for improving personal safety and building integrity across various engineering applications.

A tailor-made blue organic emitter with hot exciton and aggregation-induced emission characteristics serves as a sensitizer in the innovative sensitizing system with a dual-channel stepwise energy transfer feature. The established material and device approach enables efficient, stable blue organic light-emitting diodes with narrow emission and low-efficiency roll-off at high luminance.

Marching toward next-generation ultrahigh-definition and high-resolution displays, the development of high-performance blue organic light-emitting diodes (OLEDs) with narrow emission and high luminance is essential and requires conceptual advancements in both molecular and device design. Herein, a blue organic emitter is reported that exhibits hot-exciton and aggregation-induced emission characteristics, and use it as a sensitizer in the proposed triplet–triplet annihilation (TTA)-assisted hot-exciton-sensitized fluorescence (HSF) device, abbreviated THSF. Results show that through dual-channel stepwise Förster and Dexter energy transfer processes, the THSF system can simultaneously enhance exciton utilization, accelerate exciton dynamics, and reduce the concentration of triplet excitons. The smooth management of excitons makes the overall performance of the THSF device superior to the control TTA fluorescence and HSF devices. Furthermore, a high-performance narrowband blue (CIEx,y = 0.13, 0.12) OLED is achieved using a two-unit tandem device design, providing an excellent maximum external quantum efficiency of 18.3%, a record-high L 90% (the luminance where the ƞ ext drops to 90% of its peak value) of ≈20 000 cd m−2, and a long half-lifetime at 100 cd m−2 initial luminance of ≈13 256 h. These results showcase the great potential of the THSF strategy in realizing efficient and stable blue OLEDs with narrow emission and high luminance.

This work developed a LiC6@Li counter electrode, as an alternative to Li metal for more precisely evaluating the electrochemical behavior of electrode materials at low temperatures. The low interfacial resistances facilitate preferential de-intercalation of Li+ from LiC6, resulting in a sharp decreased over-potential at low temperatures. Meanwhile, the rapid replenishment of Li+ through the solid–solid-connection reaction maintains stable LiC6@Li potential.

Li metal, as a counter electrode, is widely used for electrode materials evaluation in coin type half-cells. However, whether this configuration is suitable for different working conditions has often been neglected. Herein, the large resistance and high cathodic/anodic over-potential of Li metal at low temperature are highlighted, revealing its incompetence as counter electrode on cryogenic condition. In view of this, a novel LiC6@Li composite electrode is developed as a promising substitution for electrode materials evaluation. In the LiC6@Li electrode, Li+ de-intercalated from LiC6 preferentially due to the low interface resistance of LiC6, presenting a cathodic/anodic over-potential of 0.05 V (67 µA cm−2) at −20 °C, which is ten times lower than that of Li metal. Moreover, the rapid lithium replenishment into LiC6 from Li metal enables a stable potential of LiC6@Li. Consequently, the LiC6@Li-based half-cells enabled more precise evaluation of the Li+ storage potential and specific capacities of a series of electrode materials at low temperature. As an extension, KC8@K is also successfully prepared as a superior counter electrode to K metal. This work proposes a suitable counter electrode for more accurately evaluating electrode materials at subfreezing scenarios, demonstrating the necessity of specialized electrode evaluation systems for particular operating conditions.

The fabricated oriented chitosan nanofibrillar hydrogels (O-CN gels), via the synergy strategy of protein templating and mechanical training, achieve cartilage-like structure and mechanical performances, as well as high-water retention similar to cartilage. The resulting O-CN gels has excellent prospects in load-bearing cartilage engineering application.

Cartilage, as a load-bearing tissue with high-water content, exhibits excellent elasticity and high strength. However, it is still a grand challenge to develop cartilage-adaptive biomaterials for replacement or regeneration of damaged cartilage tissue. Herein, protein templating and mechanical training is integrated to fabricate crystal-mediated oriented chitosan nanofibrillar hydrogels (O-CN gels) with similar mechanical properties and water content of cartilage. The O-CN gels with an ≈74 wt% water content exhibit high tensile strength (≈15.4 MPa) and Young's modulus (≈24.1 MPa), as well as excellent biocompatibility, antiswelling properties, and antibacterial capabilities. When implanted in the box defect of rat's tails, the O-CN gels seal the cartilage (annulus fibrosus) defect, maintain the intervertebral disc height and finally prevent the nucleus herniation. This synergy strategy of protein templating and mechanical training opens up a new possibility to design highly mechanical hydrogels, especially for the replacement and regeneration of load-bearing tissues.

A novel composite proton exchange membrane (PEM) design that leverages carboxylic acid-functionalized polymers of intrinsic microporosity (cPIM-1) and polyvinylpyrrolidone (PVP). Harnessing Lewis acid-base interactions enables the development of a synergistic microporous structure that confines phosphoric acid clusters, enhancing proton conductivity and durability. This work addresses critical challenges in PEM development, while proposing a solutionfor the design of next-generation membranes.

High-temperature proton exchange membrane fuel cells (HT-PEMFCs) is regarded as a promising energy conversion system owing to simplified water management and enhanced tolerance to fuel impurities. However, phosphoric acid (PA) leaching remains a critical issue, diminishing energy density and durability, posing significant obstacle to the commercial development of HT-PEMFCs. To address this, composite membranes incorporating the carboxylic acid-modified polymer of intrinsic microporosity (cPIM-1) are designed as framework polymer, blended with polyvinylpyrrolidone (PVP) for HT-PEMFCs. The Lewis acid-base interactions between cPIM-1 and PVP created an extensive hydrogen-bonding network, improving membrane compatibility. The optimized microporous structure and multiple anchoring sites gave rise to “domain-limited” PA clusters, enhancing the capillary effect. Simultaneously, improved hydrophobicity synergistically optimizes catalytic interface, promoting continuous and stable proton transfer. The HT-PEMFCs based on PVP/cPIM-1 composite membrane achieved a peak power density of 1090.0 mW cm−2 at 160 °C, representing a 152% improvement compared to PVP/PES membrane. Additionally, it demonstrated excellent durability, with a voltage decay of 0.058 mV h−1 over 210 h of accelerated stress test corresponds to more than 5000 h of constant current density durability test. This study presents a promising strategy for the development of high-performance and durable novel membranes in various energy conversion systems.

Arylboronic acids are explored for use in the electrolyte engineering of Li─S batteries. The theoretically and experimentally verified coordination and mediation chemistry of arylboronic acids can not only stabilize the anode interface but also accelerate the sluggish sulfur conversion. 3,5-bis(trifluoromethyl)phenylboronic acid (BPBA) is chosen as a suitable electrolyte modifier, significantly improving the electrochemical performance of Li─S batteries.

Lithium-sulfur (Li─S) batteries offer a promising avenue for the next generation of energy-dense batteries. However, it is quite challenging to realize practical Li─S batteries under limited electrolytes and high sulfur loading, which may exacerbate problems of interface deterioration and low sulfur utilization. Herein, the coordination and mediation chemistry of arylboronic acids that enable energy-dense and long-term-cycling Li─S batteries is proposed. The coordination chemistry between NO3 − and arylboronic acids breaks the resonance configuration of NO3 − and thermodynamically promotes its reduction on the anode, contributing to a mechanically robust interface. The mediation chemistry between lithium arylborate and polysulfides distorts S─S/Li─S bonds, alters the rate-determining step from Li2S4→Li2S2 to Li2S6→Li2S4, and homogeneously accelerates the sulfur redox kinetics. Li─S batteries using 3,5-bis(trifluoromethyl)phenylboronic acid (BPBA) show excellent cycling stability (1000 cycles with a low capacity decay rate of 0.033% per cycle) and a high energy density of 422 Wh kg−1 under aggressive chemical environments (high sulfur loading of 17.4 mg cm−2 and lean electrolyte operation of 3.6 mL gS −1). The basic mechanism of coordination and mediation chemistry can be extended to other arylboronic acids with different configurations and compositions, thus broadening the application prospect of arylboronic acids in the electrolyte engineering of Li─S batteries.

Sub-nanowires organohydrogels featuring a dual-phase structure are fabricated through the simple mixing of hydroxyapatite sub-nanowires with organic solvent and aqueous phase, directly forming a stable water-in-oil structure. The organohydrogels inherently possess rapid self-healing ability, exhibit specific temperature-responsive behavior, and are broadly compatible with a variety of organic solvents and polymers.

Organohydrogels have significant applications in numerous fields. The current synthetic strategies generally rely on the intricate and complex design of lipophilic or hydrophilic polymers to achieve the goal of oil-water interpenetration. Herein, sub-nanowires organohydrogels with a dual-phase structure are fabricated by simply mixing hydroxyapatite sub-nanowires with organic solvent and aqueous phase. The sub-nanowires in the oil phase provide structural support, while surfactants in the sub-nanowires exist at the interface between oil and water, thus forming the water-in-oil structure. The organohydrogels possess commendable mechanical properties, an inherent self-healing ability, and a specific temperature-responsive behavior. Moreover, the organohydrogels are compatible with a variety of organic solvents and polymers, reserving the promise for wide-range applications in the future.

The rational toughening of photosensitive films is crucial for the development of flexible organic solar cells. Herein, a fine-grain strengthening strategy is demonstrated for mitigating the excessive aggregation or crystallization in small-molecule acceptor films, thereby suppressing the non-ideal thermodynamic behavior and residual-enriched state. Thus, these provide the potential for the synergistic enhancement of efficiency, mechanical and environmental stability in organic photovoltaics.

The rational toughening of photosensitive films is crucial for the development of robust and flexible organic solar cells (F-OSCs), which are always influenced by mechanical strain and thermodynamic relaxation within the films. Nevertheless, the potential determinants of these properties and quantitative metrics modulating the overall performance of flexible devices have not been thoroughly defined. Herein, a fine-grain strengthening strategy is demonstrated for mitigating the excessive aggregation or crystallization in small-molecule acceptor films, the secondary thermal relaxation of side chains in polyethylene oxide (PEO) local motion restricts the free fluctuation volume through hydrogen-bonding interactions, thereby suppressing the non-ideal thermodynamic behavior and residual-enriched state. These contribute to an increase in yield strength and a reduction in microcracks while enhancing the fracture energy at the donor/acceptor interface. Finally, the optimal F-OSCs demonstrate champion PCEs of 19.12% (0.04 cm2) and 16.92% (1.00 cm2), and maintain 80% of their initial efficiency after heating at 85 °C for 2600 h. Besides, the flexibility and mechanical robustness of devices are also optimized, the elastic modulus and stiffness are decreased by 50.68% and 5.71%. This work provides interesting references for the synergistic enhancement of efficiency, mechanical and environmental stability in flexible organic photovoltaics.