Highly concentrated gel electrolytes combining polymer confinement with concentrated salt chemistry hold great promise for advanced aqueous sodium‐ion batteries (ASIBs). However, strong hydrogen‐bond self‐association in conventional protic polymers occupies functional sites and impedes effective water confinement, limiting ionic conductivity, electrochemical stability, and environmental adaptability. Herein, we design a concentrated gel electrolyte based on an aprotic poly(N,N‐dimethylacrylamide) (PDMA) matrix, which liberates abundant carbonyl sites to establish a robust and dynamically balanced polymer‐ion‐water network. Mechanistic analyses reveal that these freed C=O groups anchor H 2 O and promote anion‐participated Na + solvation, effectively restraining H 2 O activity and lowering the Na + migration barrier. These effects synergistically expand the electrochemical stability window and enable a high ionic conductivity of 43 mS cm −1 , surpassing those of reported hydrogel electrolytes (<30 mS cm −1 ). The assembled Na 3 (VOPO 4 ) 2 F@rGO//NaTi 2 (PO 4 ) 3 /C full cell achieves a high operating voltage of 2.2 V and an energy density of 61.6 Wh kg −1 (70 °C). The restrained water activity enables stable cycling from −20 to 70 °C, with the full cell retaining an energy density of 49.4 Wh kg −1 at −20 °C (85.6% of the room‐temperature value). Moreover, the elimination of interchain hydrogen bonds relaxes the polymer network, facilitating the design of a flexible pouch cell that withstands repeated bending and retains 89.8% capacity after 100 cycles under a fixed 180° bending. This work demonstrates that aprotic polymer design is an effective strategy for constructing robust solvation networks in versatile aqueous energy storage systems.
Semiconductor photocatalysis provides a sustainable route for solar‐to‐fuel conversion to mitigate global energy and environmental crises. Metal halide perovskites (MHPs) have emerged as promising photocatalysts due to their low cost, tunable compositions and band structures, excellent photoelectric properties, and scalable preparation. Nevertheless, rapid bulk charge recombination and narrow light absorption range severely restrict their photocatalytic efficiency. Fabricating S‐scheme heterojunctions has become an advanced modification strategy to accelerate charge separation and transfer while maintaining high redox potentials. This review systematically elucidates the crystal and physicochemical properties of MHPs, the evolution of S‐scheme heterojunctions, and the advantages of MHP‐based S‐scheme photocatalysts. The synthesis strategies, underlying mechanisms, and advanced characterization techniques for tracking charge behavior in such heterojunctions are summarized. Additionally, recent advances in MHP‐based S‐scheme photocatalysts are reviewed across hydrogen evolution, CO 2 photoreduction, pollutant remediation, and H 2 O 2 photosynthesis. Finally, the current challenges and future perspectives of these composite photocatalytic systems are proposed.
Integrated optoelectronic synapses that combine sensing, memory, and computation in a mechanically compliant platform are attractive for energy‐efficient wearable artificial vision and in‐sensor computing. However, simultaneously achieving intrinsic rectification, analog weight programmability, optical responsivity, and facile, scalable fabrication remains challenging. Here, we report a self‐rectifying, flexible, semi‐transparent optoelectronic memristor fabricated by layer‐by‐layer solution processing and spray coating, thereby avoiding the use of vacuum‐deposited noble‐metal top electrodes. The indium tin oxide/ZnO/TiO 2 nanosheet/MXene heterostructure uses defect‐rich ZnO as a photoactive oxygen‐vacancy reservoir, crystalline TiO 2 nanosheets (TS) as a charge‐trapping and barrier‐modulating interlayer, and a termination‐rich 2D MXene sheets (MS) electrode to promote asymmetric carrier injection. The device exhibits unidirectional analog switching with a rectification ratio of ~10 3 , stable potentiation and depression with nonlinearity values of 2.02 and 2.38, a conductance on/off ratio of 121.4, and 94.3% inference accuracy using experimentally extracted weight states. Under illumination, it shows wavelength‐selective photosynaptic behavior, stronger excitation at 365 nm, along with intensity‐ and duration‐dependent transitions from short‐term plasticity (STP) to long‐term plasticity (LTP), paired‐pulse facilitation (PPF), and learning‐forgetting‐relearning characteristics. These electrical and optoelectronic functions are preserved under bending, supporting robust mechanical reliability. Mechanistically, the response is governed by interface‐controlled barrier modulation mediated by oxygen‐vacancy redistribution, charge trapping/de‐trapping at the ZnO/TS interface, and asymmetric carrier injection at the MS/TS contact, as evidenced by postsynaptic current (PSC). This work establishes a scalable, semi‐transparent platform for energy‐efficient neuromorphic photosensing and in‐sensor wearable computing for artificial vision systems.
Mixed plastic waste remains difficult to upcycle selectively under mild conditions, and piezocatalysis has been constrained by a persistent see‐saw effect: Stronger piezoelectric polarization tends to divert charge carriers away from the very active sites that drive catalysis. Sha et al. (Nature Communications, 2026) resolve this trade‐off by substituting phosphate into BiOIO 3 nanorods, creating polarization vacancies that redirect the internal field toward exposed catalytic facets while generating frustrated Lewis acid–base pairs at the resulting I‐O‐P bonding sites. Under ultrasonic stimulation, these sites activate water and generate hydroxyl radicals that drive oxidative reforming of PET, PLA, PE, and their mixtures, achieving over 87% combined H 2 /CO selectivity and, for PET, a combined methanol/ethanol production rate of 89 mmol g −1 h −1 . By establishing polarization reorientation as a general design strategy rather than as a material‐specific fix, this work offers a transferable framework for advancing mechanically driven catalysis toward practical, ambient‐condition plastic upcycling.
Structural degradation in Li‐rich manganese‐based cathodes, driven by irreversible lattice‐oxygen loss and transition‐metal migration, remains a key obstacle to their practical deployment in high‐energy lithium‐ion batteries. Here, we report a facile oxidant‐driven strategy to reconstruct LiMn 6 superstructure units in the Li 2 MnO 3 ‐like domains of Co‐free Li 1.2 Ni 0.2 Mn 0.6 O 2 . Controlled re‐sintering with KMnO 4 treatment oxidizes a fraction of Ni 2+ to Ni 3+ , which has a similar ionic radius to Mn 4+ , partially converting LiMn 6 superstructure units into LiNiMn 5 units. Guided by Pauling's electrostatic valence principle, the LiNiMn 5 ‐containing motifs obtained through this Ni/Mn exchange mitigate the aggregation of LiMn 6 units within the Li 2 MnO 3 ‐like domains. Concurrently, the treatment induces surface‐enriched oxygen vacancies. This synergistic effect of bulk superstructure dispersion and surface oxygen‐vacancy regulation enhances oxygen redox reversibility during cycling by suppressing O–O dimerization, transition metal migration, and irreversible molecular O 2 release, thereby strengthening the layered framework's stability. As a result, the modified cathode (K‐LRM) delivers 231 mAh g −1 at 0.1 C and retains 83.8% of its capacity after 500 cycles at 1 C, with a reduced average voltage decay of 0.88 mV cycle −1 compared with 1.18 mV cycle −1 for the pristine LRM. This work demonstrates a simple and scalable route to tailor superstructure and anionic redox chemistry in Co‐free LRM cathodes, offering general guidelines for designing next‐generation high‐capacity and structurally stable layered oxides.
All‐solid‐state lithium–sulfur batteries (ASSLSBs) have emerged as a promising candidate for next‐generation energy storage systems owing to the synthetic advantages of the high energy density, low cost and abundant resources of sulfur, and the high safety merit of solid‐state electrolyte (SSE). Among the various SSEs, sulfide electrolytes occupy an important position due to their high room‐temperature ionic conductivity and superior mechanical deformability. Nevertheless, the performance of ASSLSBs with sulfide SSEs is limited by challenges associated with the sulfur cathode, such as the electronic insulating properties of sulfur, the large volume changes during charge/discharge, and the low redox dynamics of polysulfides, which are responsible for poor rate capability and unstable interfacial contact. This review systematically summarizes recent advances in sulfur cathodes for ASSLSBs: cathode design and cathode–electrolyte interfacial engineering, including component optimization, doping, catalyst incorporation, interfacial instability, and mechanical contact issues at the cathode–electrolyte interface. The effects of sulfide electrolyte types, synthesis strategies, and air/moisture hydrolysis are also discussed. Furthermore, further development of ASSLSBs is also prospected. The review may be useful for the development of ASSLSBs and other sulfur‐based solid‐state batteries such as Na/K/Zn/Mg/Ca et al.
Replacing organic liquid electrolytes with solid‐state electrolytes in all‐solid‐state batteries (ASSBs) is a highly promising strategy to increase the energy density and safety. However, issues with dendrite formation, limited Li‐ion conduction at room temperature, and poor oxidative stability of the solid‐state electrolytes severely retard the practical application of ASSBs. The present work provides a novel LiBH 4 ‐based electrolyte with a highly lithium‐ion conductive ZrB 2 network coupling with LiCl on the surface of the LiBH 4 particles by a facile mechanochemical reaction of LiBH 4 with ZrCl 4 , which results in a high ionic conductivity of 1.7 × 10 −4 S cm −1 . This network surface allows an extremely low electron conductivity and functions as a buffer zone for the deposition of metallic Li. A wide electrochemical window up to 7.0 V (vs Li/Li + ) and a high critical current density (7.2 mA cm −2 ) at 30 °C is achieved with the Li electrode. Li|LiCoO 2 and Li|TiS 2 full cells coupled with this electrolyte provide high stability at high rates, up to 3 C and 6 C, respectively. In addition, 22LiBH 4 ZrCl 4 can improve the interfacial stability against Li metal and the dendrite‐suppression capability of other solid electrolytes that are less stable toward Li or show weaker resistance to dendrite growth, such as LLZTO4LiBH 4 and Li 3 InCl 6 . Moreover, comparative studies of 22LiBH 4 ZrCl 4 and ball‐milled products derived from several other metal chlorides further confirm the structure–property relationship between the network morphology in composite solid electrolytes and their high critical current densities.
After decades of development, high‐temperature superconductors are undergoing an important stage from laboratory research to practical applications. Among all candidates, LRE 1+ x Ba 2− x Cu 3 O 7− δ (LRE123, LRE for light rare‐earth elements) oxides possess outstanding critical transition temperatures and high critical current densities. However, like many functional materials, LRE123 superconductors greatly suffer from cation off‐stoichiometry resulting from the LRE 3+ /Ba 2+ substitution, which adversely affects their performance. Recently, it is found that the cooling rate, as a decisive factor of crystallization, also serves as a powerful tool for regulating the oxygen vacancy and further managing cation stoichiometry. This paper provides an overview of the newly reported cooling‐rate‐control melt‐growth of LRE123 bulks with high superconducting performance. The underlying mechanism correlated with superconducting properties is comprehensively elucidated.
Silver‐based nanostructures are widely believed as the promising catalysts for electrocatalytic reduction of carbon dioxide toward carbon monoxide. However, most reported Silver‐based catalysts are typically synthesized in powder form and require polymeric binders for electrode fabrication, resulting in several interrelated issues including blocked active sites, poor electrical conductivity, limited mass transport, and weak adhesion between the catalyst layer and the substrate. Herein, utilizing a three‐dimensionally porous anodic aluminum oxide template, a self‐supported 3D interconnected Ag nanowire membrane is fabricated as a electrocatalytic reduction of carbon dioxide electrode. This unique architecture offers a large electrochemical active surface area and abundant active sites, enabling the efficient and highly selective conversion of carbondioxide to carbon monoxide over a wide potential window, with a maximum Faradaic efficiency for carbon monoxide of 97.28% and high current density of 59.06 mA cm −2 in the typical H‐type cell. Furthermore, the scaffold‐like 3D interconnected structure ensures excellent structural stability, guaranteeing long‐term operational durability. This work provides a novel catalyst design strategy for highly selective electrocatalytic reduction of carbon dioxide to carbon monoxide and a feasible solution for durable self‐supporting electrodes.
Introducing ferroelectric spontaneous polarization (Ps) electric field to suppress the recombination of photogenerated carriers is crucial for enhancing catalytic activities. Herein, we report a strategy to effectively facilitate the ferroelectricity and charge carrier behavior by compositing MAPbI 3 with hydroxyl‐containing (EOA) 2 PbBr 4 . Density functional theory calculations reveal that the hydroxyl groups will alter the orientation of polar MA + ions, leading to a more uniform alignment with the polarization direction in MAPbI 3 . The ferroelectric‐related piezoelectric constant and spontaneous electric potential demonstrate significant improvements, reaching 43.81 pm V −1 and −876.2 mV, respectively, as measured by piezoresponse force microscopy and kelvin probe force microscope. Furthermore, the increase in the intensity of the steady‐state surface photovoltage (SPV) signal and the slow attenuation of the transient SPV signal in (EOA) 2 PbBr 4 /MAPbI 3 indicate an enhanced Ps electric field, enabling desirable spatial separation of photogenerated carriers. Moreover, photocatalytic CO 2 reduction shows that the CO production rate of the (EOA) 2 PbBr 4 /MAPbI 3 reached 90.37 μmol g −1 , representing a 2.5‐fold increase compared to MAPbI 3 . Overall, this work presents a novel approach to designing high‐performance halide perovskite photocatalytic materials by manipulating ferroelectricity effects through functional groups.
The increasing demand for efficient thermal energy storage systems has driven the development of phase change material microcapsules (PCMMs), which provide high energy‐storage density, reversible phase change, and reduced leakage. Conventional microencapsulation methods for phase change materials (PCMs) (e.g., coacervation, solvent evaporation, and spray drying) suffer from limitations such as the use of toxic reagents, poor mechanical stability, and leakage. In contrast, the Pickering emulsion templating method employs solid nanoparticles to stabilize PCM‐based emulsions, followed by polymerization of organic monomers or inorganic precursors at the oil–water interfaces to create shells, enabling greener processing, higher encapsulation efficiency, superior mechanical and thermal robustness, and tunable shell properties. This review systematically examines the workflow of PCMM fabrication via the Pickering emulsion templating method, covering: 1) PCM classification, phase change mechanisms, and thermal properties; 2) preparation of PCM‐based Pickering emulsions; 3) formation of microcapsule shells; and 4) post‐treatments. The underlying structure–property relationships are also evaluated to clarify the impact of architectural design on thermal storage capacity and mechanical durability. Subsequently, a critical review of their utility in several application fields, such as energy devices and flexible electronics, functional fibers and smart coatings, building materials and cryogenic transportation, environmental remediation, and drug delivery, is provided. Finally, current challenges and future directions are discussed to guide translation into practical thermal energy applications.
Organic semiconductor single crystals (OSSCs) represent a critical materials platform for pushing the performance limits of organic optoelectronic devices, owing to their structural perfection, absence of grain boundaries and ultralow trap densities. Among existing growth methods, gas–solid interface‐assisted growth strategy stands out, due to its superior advantages in controlling the dimension, morphology, structure, and orientation of OSSCs. Recent breakthroughs demonstrate that precise manipulation of nucleation and growth dynamics, through tailored temperature, carrier gas engineering, interface modification and molecular component optimization, enables the reproducible preparation of high‐quality OSSCs at gas–solid interface. This review provides a comprehensive overview of the fundamental principles and state‐of‐the‐art gas–solid interface‐assisted growth strategies. It critically examines the relationship between growth parameters and resulting crystal properties, highlights representative high‐performance devices based on such crystals, and outlines key challenges and outlooks for advancing this approach toward high‐performance organic optoelectronics.
Vapor accumulation often limits the performance of passive interfacial solar evaporation. Inspired by the Dyson sphere concept, Xu, Yang, and co‐workers designed a perforated‐shell evaporator with an internal non‐evaporating core that diverts incident sunlight to drive self‐generated internal convection for vapor removal. This strategy provides a versatile pathway for enhancing interfacial mass transfer in sustainable solar to water technologies.
Developing self‐powered photodetectors capable of processing multidimensional optical signals is pivotal for next‐generation photonic computing and secure communications. However, conventional device architectures are typically limited to single‐mode intensity detection, and the complex photophysics within coupled photovoltaic units remain poorly understood. Here, we reveal a unified “Photovoltaic‐Capacitance” coupling mechanism within a vertically stacked, self‐powered Ga 2 O 3 /PEDOT:PSS and ZnO/Graphene architecture. We demonstrate that the system's wavelength‐selective, transient bipolar response is governed by the multifaceted charging and discharging dynamics between the two coupled units. The key to this mechanism is the ZnO/Graphene (3D/2D) interface, which we define as a novel “Photovoltaic Dynamic‐Capacitor” (PDC) component, exhibiting a defined four‐stage transient (instantaneous polarization, steady‐state saturation, reverse discharge, and relaxation). This architecture enables the Ga 2 O 3 unit (photovoltaic source) to dynamically charge the PDC under 270 nm illumination (+0.27 A/W), while 380 nm illumination directly activates the PDC itself, generating a reverse current (−0.009 A W −1 ). This universal (proven with MgZnO) and dynamically coupled architecture establishes a viable approach for self‐powered, multidimensional optical processing. We leverage this unique behavior to implement a physical layer secure communication protocol based on an innovative ternary optical logic (“1”, “0”, “−1”), offering enhanced anti‐jamming capabilities rooted in a new photonic degree of freedom.
Driven by the growing demand for next‐generation high‐energy‐density energy storage systems, conversion‐type cathodes have emerged as promising candidates for lithium metal batteries (LMBs) owing to their multi‐electron redox chemistry and ultrahigh theoretical capacities. However, their practical application is hindered by sluggish kinetics, severe structural degradation and active material dissolution, which are closely associated with complex phase evolution and unstable electrode–electrolyte interfaces. Electrolyte engineering has emerged as a critical strategy to address these challenges, primarily by tailoring the Li + solvation structure to regulate interfacial reactions and reaction pathways. This review provides a comprehensive overview of recent advances in electrolyte design for conversion‐type cathodes, including conventional electrolytes, high‐concentration electrolytes (HCEs), localized HCEs (LHCEs), weakly solvating electrolytes (WSEs), additive‐engineered systems, and ionic liquid electrolytes (ILEs). Particular emphasis is placed on the correlation among Li + solvation structures, interfacial chemistry, and overall electrochemical performance. Finally, the remaining challenges and future perspectives for rational electrolyte design toward practical, high‐energy‐density conversion‐type cathodes‐based LMBs are outlined.
Architecting nanometric cluster electrocatalysts with high density of active atoms offers a valuable avenue to simultaneously augment atomic utilization efficiency and catalytic stability. Herein, nanometric IrO x and RhO x clusters are anchored onto the spinel Co 3 O 4 framework (CoMO x , M = Ir, Rh), yielding a unique amorphous/crystalline heterostructure. The optimized CoMO x catalysts with precise‐tuning calcination treatment present a favorable electrocatalytic activity with low OER (CoIrO x : 235 mV @ 10 mA cm −2 ) and HER (CoRhO x : 157 mV @ 10 mA cm −2 ) overpotentials. Operando electrochemical impedance spectroscopy in combination with density functional theory calculations reveal that the strong interfacial electronic coupling between nanometric clusters and the spinel Co 3 O 4 matrix enhances the electron density near the Fermi level and upshifts the d‐band center, thereby facilitating hydrogen release during the HER and lowering the OER rate‐determining step (OH*→O*) free energy.
Hydrogen peroxide (H 2 O 2 ) is a vital oxidant with broad industrial applications, and its production via photocatalysis represents a highly promising approach. Titanium dioxide (TiO 2 ) has garnered significant attention for photocatalytic H 2 O 2 generation. In this study, a simple method was used to enhance the photocatalytic performance by loading juglone as a co‐catalyst onto anatase TiO 2 . The quinone group of juglone serves as an efficient electron acceptor, effectively capturing conduction band electrons from TiO 2 to form stable semiquinone radical anions. Simultaneously, the phenolic hydroxyl group acts as a hole‐trapping site, promoting hole migration to the surface. This dual‐pathway charge separation mechanism substantially suppresses electron–hole recombination and improves quantum efficiency. Consequently, under illumination, the Juglone/TiO 2 photocatalyst achieved an H 2 O 2 production rate of 5851.44 μmol g −1 h −1 in an aqueous benzyl alcohol (as the hole scavenger) solution under an air atmosphere within 1 h. This work offers a new strategy for developing efficient and stable catalysts for solar fuel production.
The rapid development of flexible electronics has imposed demands on the comprehensive properties of conductive materials.This paper systematically reviews the synergistic design strategies of conductive nanocomposites based on zero-dimensional(0D),one-dimensional(1D),and two-dimensional(2D)nanomaterials,covering their preparation methods,synergistic mechanisms,electronic and mechanical properties,and cutting-edge applications in flexible electronics.By integrating the high electrical conductivity of 0D nanoparticles,the strain dissipation ability of 1D nanostructures,and the chemical stability and interfacial charge transfer of 2D materials,multi-dimensional synergistic effects can be achieved through strategies such as multi-dimensional spatial structure regulation and interface engineering,thereby overcoming the performance limitations of single-type materials.These effects enable a balance of electrical conductivity,flexibility,and stability via spatial complementarity of materials with different dimensions(0D filling,1D bridging,2D support),interface optimization(quantum confinement effect,van der Waals force regulation),and functional integration.This review establishes a universal design principle for the rational design of multi-dimensional conductive nanomaterials for flexible electronics.
The pursuit of safer and higher energy‐density batteries has positioned all‐solid‐state lithium batteries (ASSLBs) at the forefront of next‐generation energy storage technologies. The solid‐state electrolyte (SSE) serves as the pivotal component, with its thin‐film fabrication being critical for minimizing inactive material mass and maximizing energy density—a decisive step toward commercial viability. However, the transition from fundamental materials discovery to high‐performance, ultrathin SSE membranes faces significant challenges, including insufficient ionic conductivity, poor interfacial stability, and inadequate mechanical integrity at reduced dimensions. This review provides a comprehensive overview and critical analysis of the latest advancements in the design and manufacturing of thin‐film composite SSEs. We first delineate the intrinsic limitations of conventional inorganic and polymer SSEs, establishing the imperative for composite strategies. The core of the review systematically navigates advanced fabrication methodologies—spanning wet, dry, and emerging processes—and architectural innovations, with a focus on nanofiller engineering, layered structures, and 3D scaffolds. We emphasize the synergistic interplay between processing techniques and multiscale structures in simultaneously enhancing ionic transport, mechanical robustness, and electrode compatibility. By framing a comprehensive “processing–structure–performance” paradigm, this review aims to guide future research endeavors and accelerate the development of industrially relevant thin‐film SSEs for practical high‐energy‐density ASSLBs.
With the rapid growth of the global lithium‐ion battery‐powered electric vehicle (EV) market, their overall sustainability becomes an emerging concern. This work reviews the most up‐to‐date literature and provides our own critical analysis and perspectives. The topics covered by this study include resource sustainability and greener manufacturing of lithium‐ion batteries, greenhouse gas and air pollutant emissions of electric vehicles, and the impact of electric vehicle charging on the power grid. Briefly, the raw materials face low supply risks as the cathodes switch to low cobalt scenarios. For the greenhouse gas emissions, we first derive the equations for calculation of emissions from vehicle production, lithium‐ion battery production, and the electric vehicle use phase. Subsequently, a heuristic‐based method is adopted to determine the parameters and coefficients, while an Excel spreadsheet is created for facile calculations of the GHG emissions. This spreadsheet is included in the for free download and use. The benefits of greenhouse gas and air pollutant emission reduction for electric vehicles are obvious compared to internal combustion engine vehicles. In the future, these benefits will be further augmented by grid electricity decarbonization and deployment of more effective end‐of‐pipe air pollutant control measures. The charging of electric vehicles poses negative impacts on the stability of the power grid. However, if managed properly, these impacts can be effectively mitigated; moreover, EVs can even promote renewable electricity incorporation. Furthermore, this study summarizes greener manufacturing practices in lithium‐ion battery production, which are beneficial for both resource sustainability and life‐cycle emission reduction of electric vehicles.
