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

Herein, a novel inorganic/organic hybrid hydrogel electrolyte is prepared via in situ sol-gel polymerization. A high ion conductivity is achieved even under a lean-water condition. Abundant polar functional groupstend to form hydrogen bonds with water molecules, thereby reducing the hydrogen evolution reaction. This hydrogel electrolyte exhibits excellent performance in both symmetrical Al batteries and full batteries.

Rechargeable aqueous aluminum ion batteries (AAIBs) offer a promising avenue for achieving safe, high-energy, and low-cost large-scale energy storage applications. However, the practical development of AAIBs is hindered by competitive reduction reactions in the aqueous solution, which lead to insufficient aluminum (Al) deposition and a severe hydrogen evolution reaction (HRE). In this work, an inorganic/organic hybrid hydrogel with a stable silicon-based network and multiple polar sites is successfully fabricated via an in situ sol-gel polymerization method. The preferential formation of hydrogen bonds between the polar functional groups and water molecules effectively reduces the thermodynamic reactivity of water. Furthermore, X-ray photoelectron spectroscopy (XPS) and time of flight secondary ion mass spectrometry (TOF-SIMS) analyses confirm the formation of a stable, inorganic-rich solid electrolyte interface (SEI) layer, which kinetically suppresses undesirable side reactions. This hydrogel electrolyte exhibits a high ionic conductivity of 2.9 × 10−3 S cm−1 at 25 °C, even under lean-water conditions. As a result, Al|hydrogel|potassium nickel hexacyanoferrate (KNHCF) full cells demonstrate excellent cycling performance, delivering a high initial discharge capacity of 74.9 mAh g−1 at 100 mA g−1 and achieving an outstanding capacity retention of 90.0% after 200 cycles. Additionally, pouch cells exhibit stable open-circuit voltage under various mechanical abuse conditions.

Critical ingredients can revitalize magnesium-metal anode in conventional electrolytes. Mechanistic insights, with an emphasis on Mg-ion solvation structure regulation, interfacial evolution, solvent ionization, and weak interfacial passivation, have been especially underscored in terms of the close relationship between electrolyte chemistries and weakly-passivated interphase properties.

Multivalent-metal batteries hold tremendous promise in solving safety and sustainability problems encountered by common lithium-ion batteries, but the lack of ideal electrolyte solutions restricts their large-scale adoption. Tuning electrolyte structures with functional ingredients, especially amines/methoxy-based amines and phosphates, can revitalize multivalent-metal anodes and high-voltage cathodes in conventional electrolytes, unlocking their full potential. However, a rational and clear understanding of the implications of these ingredients, notwithstanding critically important to commercially available electrolyte design, has not been widely accepted. This concise perspective aims to provide timely analysis and discussion on ingredients’ functionalities of solvation shell speciation, interphase evolution, and consequently metal plating/stripping kinetics acceleration. In addition to prevailing coordination interactions, fresh understandings of intermolecular ionization/association and unique interphase formation are underscored by the close relationship between electrolyte chemistries and weakly passivated interphase properties. The existing understandings and proposed outlooks are expected to promote the next breakthroughs for rechargeable multivalent-metal batteries.

The incorporation of a tetrahedral Cu(I) single site into the bipyridine-based covalent organic framework (COF) is shown to effectively drive photocatalytic carbon–carbon bond formation through simultaneous energy and electron transfer pathways. The COF-based photocatalyst demonstrates efficient and durable performance for the preparation of a series of oxindole and isoindolinones.

The isoindolinone scaffold is an important structural motif found in a wide range of naturally occurring and synthetic biologically active compounds. However, the synthesis of isoindolinone derivatives typically requires multi-step procedures or the use of palladium-based catalysts, which are often hampered by low reaction yields and high costs. Recently, covalent organic frameworks (COFs)—emerging crystalline and porous materials—have gained considerable attention for their applications in various organic transformations, particularly in C─H functionalization, cross-coupling and redox reactions. Although COFs have been extensively studied for photocatalysis, the development of sustainable heterogeneous catalysts using low-cost transition metal-based photosensitizers is still in its early stages. Herein, a strategy is presented to incorporate a copper-Xantphos complex with a tetrahedral Cu(I) geometry into a crystalline and porous COF matrix. This modification enables unprecedented simultaneous electron and energy transfer efficiency during photocatalysis. The Cu–Xantphos coordinated COF exhibits potent photocatalytic activity for the synthesis of isoindolinone derivatives via C─Br and C─H bond cleavage followed by C─C bond formation. In addition, the catalyst shows excellent recyclability as it can be rejuvenated by reintroducing the Cu–Xantphos complex after multiple photocatalytic cycles—highlighting its potential as a sustainable and cost-effective solution for valuable organic transformations.

In the design of smart materials based on active agents or microswimmers, the gaits or motile states of the agents are to be controlled, preferably by external parameters that do not require modifying the composition of the system. A facile, universal parameter is temperature. Here, in the experimental model system of self-propelling active emulsions, a temperature sensitive mixture of co-surfactants is used as fuel for propulsion. It is demonstrated that three distinct states of reorienting, then straight motion, and subsequent arrest, can be accessed, counterintuitively, with increasing temperature.

Self-propelling active matter relies on the conversion of energy from the undirected, nanoscopic scale to directed, macroscopic motion. One of the challenges in the design of synthetic active matter lies in the control of dynamic states, or motility gaits. Here, an experimental system of self-propelling droplets with thermally controllable and reversible dynamic states is presented, from unsteady over meandering to persistent to arrested motion. These states are known to depend on the Péclet number of the molecular process powering the motion, which can now be tuned by using a temperature sensitive mixture of surfactants as propulsion fuel. The droplet dynamics are quantified by analyzing flow and chemical fields for the individual states, comparing them to canonical models for autophoretic particles. In the context of these models, in situ, the fundamental first broken symmetry that translates an isotropic, immotile base state to self-propelled motility, is experimentally demonstrated.

Colored radiative cooling (CRC) has become a prevailing technology for achieving colorful appearance and simultaneously enhancing the effective solar reflectance of cooling coatings. This review presents recent advancements in CRC and its profound impact on energy savings in real-world applications. After introducing the fundamentals of CRC and color characterization methods, it reviews CRC coloration approaches, including photonic structural colors, complementary color absorption and Purcell-enhanced fluorescent colors. The review concludes with self-adaptive CRC materials featuring dynamic optical modulation and their potentially practical applications as well as critical challenges.

Radiative cooling technology is gaining prominence as a sustainable solution for improving thermal comfort and reducing energy consumption associated with cooling demands. To meet diverse functional requirements such as aesthetics, switchable cooling, camouflage, and colored smart windows, color is often preferred over a white opaque appearance in the design of radiative cooling materials. Colored radiative cooling (CRC) has emerged as a prevailing technology not only for achieving a colorful appearance but also for increasing the effective solar reflectance to enhance cooling performance (through the incorporation of fluorescent materials). This paper reviews recent advancements in CRC and its profound impact on energy savings and real-world applications. After introducing the fundamentals of CRC and color characterization, various photonic approaches are explored that leverage resonant structures to achieve coloration in radiative cooling, comparing them with conventional coloration methods based on optical materials like fluorescent pigments that can convert absorbed ultraviolet light into visible-light emission. Furthermore, the review delves into self-adaptive CRC materials featuring dynamic optical modulation that responds to temperature fluctuations. Lastly, the potential application of CRC materials is assessed, a comprehensive outlook on their future development is offered, and the critical challenges in practical applications are discussed.

Heterostructures have emerged as advanced electrocatalysts to convert earth-abundant simple molecules into high-value-added products. On the basis of atomistic understanding to accelerate the electrochemical processes, the architecture of heterostructured electrocatalysts is comprehensively discussed from the point of view of modulating electronic configuration and interface reactive microenvironment. The influence of rectification, space charge region, built-in electric field, synergistic interactions, lattice strain, and geometric effect is considered.

Electrocatalysts can efficiently convert earth-abundant simple molecules into high-value-added products. In this context, heterostructures, which are largely determined by the interface, have emerged as a pivotal architecture for enhancing the activity of electrocatalysts. In this review, the atomistic understanding of heterostructured electrocatalysts is considered, focusing on the reaction kinetic rate and electron configuration, gained from both empirical studies and theoretical models. We start from the fundamentals of the microkinetic model, adsorption energy theory, and electric double layer model. The importance of heterostructures to accelerate electrochemical processes via modulating electron configuration and interfacial reactive microenvironment is highlighted, by considering rectification, space charge region, built-in electric field, synergistic interactions, lattice strain, and geometric effect. We conclude this review by summarizing the challenges and perspectives in the field of heterostructured electrocatalysts, such as the determination of transition state energy, their dynamic evolution, refinement of the theoretical approaches, and the use of machine learning.

A halogen bond (XB)-enhanced strategy is proposed, where ─B(OH)I3 groups are incorporated into a highly integrated porous carbon/I2 cathode (HOCF–BIn) to extend interactions between ─B(OH)I3 and subsequent I2 molecules. The strong intermolecular forces in HOCF–BIn cathodes significantly enhance I2/I3 −/I− confinement, enabling exceptional cycling stability at I2 loadings of 1.8–6.2 mg cm−2.

The redox chemistries of iodine have attracted tremendous attention for charge storage owing to their high theoretical specific capacity and natural abundance. However, the practical capacity and cycle life are greatly limited by the active mass loss originating from the dissolved iodine species in either non-aqueous or aqueous batteries. Despite intensive progress in physical and physicochemical confinements of iodine species (I2/I3 −/I−), less attention has been paid to confining iodine species beyond the host–iodine interface, inhibiting further development of iodine cathodes with high I2 contents. Here a halogen bond (XB)– enhanced design concept is proposed between I2 molecules to achieve stable cycling performances, as exemplified by the Na–I2 battery. The enhanced XB is derived from the incorporation of –B(OH)I3 groups in highly integrated porous carbon/I2 cathode (HOCF–BIn), which can generate extended interactions between –B(OH)I3 and following I2 molecules. Due to the strong intermolecular force between I2 molecules, the HOCF–BIn cathodes exhibit substantially strengthened I2/I3 −/I− confinement, enabling outstanding cycling stability at I2 loading ranging from 1.8 to 6.2 mg cm−2. This findings demonstrate a functional group to manipulate XB chemistry within I2 molecules and polyiodides for stable and low-cost metal–iodine batteries.

The nanoplatform based on engineered attenuated OMVs has good biosafety and can cross the BBB and target GBM with the assistance of Angiopep-2. The co-delivery of doxorubicin and CD47-siRNA and the immunogenicity of OMVs synergistically overcome the intrinsic and adaptive immune resistance of GBM, which ultimately triggers a powerful antitumor immune response.

Apart from the blood-brain barrier (BBB), the efficacy of immunotherapy for glioblastoma (GBM) is limited by the presence of intrinsic and adaptive immune resistance, implying that co-delivery of various immunotherapeutic agents or simultaneous regulation of different cells is urgently needed. Bacterial outer membrane vesicles (OMVs) offer a unique advantage in the treatment of GBM, owing to their multifunctional properties as carriers and immune adjuvants and their ability to cross the BBB. However, traditional OMVs can lead to toxic side effects and disruption of tight junctions in the BBB. Therefore, to enhance the in vivo safety and targeting capability of OMVs, we introduced engineered OMVs to reduce toxicity and further constructed a modularly assembled nanoplatform by performing simple peptide modifications. This nanoplatform demonstrates satisfactory biosafety and is able to continuously cross the BBB and target GBM with the assistance of Angiopep-2. Subsequently, immunogenic substances on OMVs, along with carried small-interfering RNA (siRNA) and doxorubicin, can promote and enhance the reprogramming and phagocytic abilities of macrophages and microglia, respectively, and increase the immunogenicity of GBM, ultimately overcoming GBM immune resistance to enhance the efficacy of immunotherapy. This OMVs-based nanoplatform provides a new paradigm and insights into the development of immunotherapy for GBM.

This review probes recent advancements in PEMWEs for green hydrogen production from the perspective of acidic OER, identifies challenges related to corrosive environments and oxidative conditions, and proposes strategies to enhance the long-term stability of PEMWEs by addressing both catalyst and membrane electrode assembly deactivation.

Proton exchange membrane water electrolysis (PEMWE) represents a promising technology for renewable hydrogen production. However, the large-scale commercialization of PEMWE faces challenges due to the need for acid oxygen evolution reaction (OER) catalysts with long-term stability and corrosion-resistant membrane electrode assemblies (MEA). This review thoroughly examines the deactivation mechanisms of acidic OER and crucial factors affecting assembly instability in complex reaction environments, including catalyst degradation, dynamic behavior at the MEA triple-phase boundary, and equipment failures. Targeted solutions are proposed, including catalyst improvements, optimized MEA designs, and operational strategies. Finally, the review highlights perspectives on strict activity/stability evaluation standards, in situ/operando characteristics, and practical electrolyzer optimization. These insights emphasize the interrelationship between catalysts, MEAs, activity, and stability, offering new guidance for accelerating the commercialization of PEMWE catalysts and systems.

A sustainable Zn interfacial architecture is established, where a robust polyimide nanofilm is covalently anchored to the Zn substrate through electronegative F atoms. The strong covalent interactions provide excellent interfacial adhesion during repeated Zn/Zn2+ cycling. The remarkable resilience, modulus, and low creep of FPI film effectively resist the impact stress from electroplated Zn while maintaining structural integrity.

Artificial interfacial protective coatings (IPCs) on Zn anodes provide a viable solution for suppressing dendritic growth by spatially confining and homogenizing the Zn2+ flux. However, repeated Zn deformation during electroplating/stripping cycles can lead to the rupture or exfoliation of IPCs, as well as the formation of detrimental interfacial gaps. Herein, a highly durable IPC is developed on a Zn substrate using a mechanically robust fluorinated polyimide nanofilm (FPI). This unique FPI interphase forms strong covalent bonds with Zn through electronegative fluorine atoms, facilitating Zn plating/stripping while maintaining interfacial adhesion. The superior resilience, modulus, and low creep of the FPI film resist the impact stresses from electroplated Zn, ensuring structural integrity. With this FPI coating, the FPI-Cu||Zn half cells demonstrate high reversibility in Zn2+ electroplating/stripping over 4000 h, maintaining Coulombic efficiency above 99.33%. When coupled with a MnO2 cathode, the MnO2||FPI-Zn full cells exhibit a long lifespan, surpassing 5000 cycles, with a high specific capacity retention of 75.21%. This study highlights the importance of achieving a balance between the customized compatibility and mechanical properties of IPCs to modulate zinc interfacial chemistries.

An infrared-sensitive image sensor based on self-welded tellurium (Te) nanomesh is proposed, demonstrating advancements in flexible integration and scalable fabrication. By leveraging the unique photothermolelectric (PTE) operation, thermal-coupled bi-directional photoresponse is explored to illustrate the proof-of-principle in-sensor convolutional network for edge computing.

The inherent limitations of traditional von Neumann architectures hinder the rapid development of internet of things technologies. Beyond conventional, complementary metal-oxide-semiconductor technologies, imaging sensors integrated with near- or in-sensor computing architectures emerge as a promising solution. In this study, the multi-scale van der Waals (vdWs) interactions in 1D tellurium (Te) atomic chains are explored, leading to the deposition of a photothermoelectric (PTE) Te nanomesh on a polymeric polyimide substrate. The self-welding process enables the lateral vapor growth of a well-connected Te nanomesh with robust electrical and mechanical properties, including a PTE responsivity of ≈120 V W−1 in the infrared light regime. Leveraging the PTE operation, the thermal-coupled bi-directional photoresponse is investigated to demonstrate a proof-of-principle in-sensor convolutional network for edge computing. This work presents a scalable approach for assembling functional vdWs Te nanomesh and highlights its potential applications in PTE image sensing and convolutional processing.

A D–A–D type TADF molecule, TPA-DHAQ, is designed and synthesized by introducing an ESIPT-active molecule DHAQ as the acceptor unit, based on which the NIR TADF laser with a low threshold and high stability is successfully realized. In addition, a single-mode NIR TADF laser can be realized by adjusting the size of the resonator. This work provides a novel molecular design strategy to overcome the problem of poor stability of conventional NIR organic lasers.

Near-infrared (NIR) organic lasers have undergone rapid development in recent years, but still facing challenges in lowering the threshold and improving the stability. Herein, to overcome these challenges, a “two in one” strategy involving the integration of thermally activated delayed fluorescence (TADF) and excited-state intramolecular proton transfer (ESIPT) activity in a single molecule is proposed. Specifically, a donor–acceptor–donor type TADF material 2,6-bis[4-(diphenylamino)phenyl]-1,5-dihydroxyanthraquinone (TPA-DHAQ) with an ESIPT-active moiety as the acceptor, is designed and synthesized, based on which, a NIR organic laser at 820 nm with an exceptionally low threshold of 6.3 µJ cm−2 can be realized. Benefiting from the synergistic effect of the TADF property and the ESIPT process, the resulting organic laser showed excellent stability by maintaining the laser intensity at ≈80% of the initial value after 580 min of continuous excitation. Finally, by modulating the size of the resonator, a single-mode NIR laser is successfully realized. This work provides a novel molecular design strategy for the development of new TADF gain materials to overcome the problem of high threshold and poor stability of conventional NIR organic lasers, and shed light on the future development of NIR organic lasers.

Meter-scale MXene/GO@monstera nanocellulose core-shell nanofiber textiles are produced, integrating ultra-broadband EMI shielding covering GHz and THz bands, super-strong stealth properties within NIR and MIR ranges, and excellent multifunctionality, including heat resistance, flame retardant, joule heating, and stress sensing capabilities, which are promising for comprehensive electromagnetic defense in both military and civilian fields.

The rapid development of wireless communication and infrared (IR) detection technologies has generated an increasing demand for large-size high-performance wearable electromagnetic interference (EMI) shielding and IR stealth textiles. Herein, meter-scale MXene/graphene oxide (MG)@monstera nanocellulose (MC) core-shell nanofiber textiles are fabricated for the first time using a multi-stage cryogenic drying-assisted coaxial wet spinning assembly strategy, with MG as the conductive composite core and MC as the organic skeleton shell. The highly aligned shell and dense core endow the nanofibers with a great toughness of ≈39.6 MJ m−3, a strong strength >≈180 MPa, and a high conductivity of 6.4 × 103 S m−1. The textiles exhibit unprecedented ultra-broadband EMI shielding performance covering gigahertz and terahertz bands, with optimal shielding effectiveness up to 84 and 85 dB in the band of 8.2–26.5 GHz and 0.3–1.5 THz, respectively, at only 185 µm thick. Superb IR stealth performance in the near- and mid-IR ranges is also achieved, benefitting from their good heat resistance and low IR emissivity. Furthermore, the textiles also demonstrate excellent dyeability, flame retardancy, Joule heating, and stress-sensing properties. Such scalable prepared core-shell nanofiber textiles with superior comprehensive performance have broad application prospects in future smart wearable protective devices.

Novel polyimide-ionene hybrids that exhibit desirable alcohol processability, conductivity, transparency, and metal/semiconductor interface modification ability are furnished by melding pyromellitic diimides into ionene backbones. These merits render them universal cathode interlayer materials with outstanding thickness tolerance, leading to not only highly efficient and stable opaque devices but also high-performance semitransparent devices even when pairing with low-cost Cu electrodes.

The contradiction between high transmittance and favorable conductivity poses a great challenge in developing effective cathode interlayer (CIL) materials with sufficient thickness tolerance, which hinders the further advancement of organic solar cells (OSCs). Herein, a completely new class of alcohol processable polyimide-ionene hybrids (PIIHs) is proposed by melding pyromellitic diimide (PMD) subunits into imidazolium-based ionenes backbone covalently. These PIIHs, named PMD-DI and PMD-PD, boast high transparency, suitable energy levels, and decent conductivity. A higher PMD content endows PMD-PD with improved work function tunability, electrical properties, and crystallinity, enabling PMD-PD as CIL material with excellent thickness-insensitive characteristics, while simultaneously improving device stability significantly. Furthermore, PMD-PD also exhibits good compatibility with various electrodes and active layers, offering solar cell efficiencies of up to 19.91% and 19.29% with Ag and Cu cathodes, respectively. More importantly, the application of PMD-PD can improve the performance of semi-transparent OSCs without losing transmittance, thereby drastically enhancing the light utilization efficiency to 4.04% with an ultrathin, low-cost Cu cathode, that competes with leading optical modulation-free semitransparent OSCs with expensive Ag cathodes. This work opens a pathway to realize transparent and conductive interlayers by strategic molecular design, leading to highly efficient, stable, and cost-effective OSCs suitable for diverse applications.

Biological nanopores are highly promising tools for single-molecule biosensors, but the fragile supporting lipid membranes is a major bottleneck. An alternative hybrid membrane is presented, comprising phospholipids and block co-polymers, that can be functionalized by a broad variety of nanopores for single-molecule sensing. Crucially, the hybrid membrane provides substantially increased stability to harsh conditions, providing new opportunities for nanopore-based biosensors.

Biological nanopores are powerful tools for single-molecule detection, with promising potential as next-generation biosensors. A major bottleneck in nanopore analysis is the fragility of the supporting lipid membranes, that easily rupture after exposure to biological samples. Membranes comprising PMOXA-PDMS-PMOXA (poly(2-methyloxazoline-b-dimethylsiloxane-b-2-methyloxazoline)) or PBD-PEO (poly(1,2-butadiene)-b-poly(ethylene oxide)) polymers may form robust alternatives, but their suitability for the reconstitution of a broad range of nanopores has not yet been investigated. Here, PBD-PEO membranes are found to be highly robust toward applied voltages and human serum, while providing a poor environment for nanopore reconstitution. However, hybrid membranes containing a similar molar ratio of PBD11PEO8 polymers and diphytanoyl phosphatidylcholine (DPhPC) lipids show the best of both worlds: highly robust membranes suitable for the reconstitution of a wide variety of nanopores. Molecular dynamics simulations reveal that lipids form ≈12 nm domains interspersed by a polymer matrix. Nanopores partition into these lipid nanodomains and sequester lipids, possibly offering the same binding strength as in a native bilayer. Nanopores reconstituted in hybrid membranes yield efficient sampling of biomolecules and enable sensing of high concentrations of human serum. This work thus shows that hybrid membranes functionalized with nanopores allow single-molecule sensing, while forming robust interfaces, resolving an important bottleneck for novel nanopore-based biosensors.

Zinc anodes face severe instability under extreme conditions of high current density, high areal capacity, and high depth of discharge (DOD) due to severe concentration polarization caused by the imbalance between Zn2⁺ consumption and transfer rates. To overcome this, a nanofluid layer is introduced to rapidly absorb Zn2⁺ and regulate interfacial ion transport, effectively mitigating polarization and enabling stable zinc deposition. This work provides key insights into interfacial engineering for next-generation high-performance zinc metal batteries.

The commercialization of zinc metal batteries aims at high-rate capability and lightweight, which requires zinc anodes working at high current density, high areal capacity, and high depth of discharge. However, frequent zinc anode fades drastically under extreme conditions. Herein, it is revealed that the primary reason for the anode instability is the severe concentration polarization caused by the imbalanced consumption rate and transfer rate of Zn2+ under extreme conditions. Based on this finding, a nanofluid layer is constructed to rapidly absorb Zn2+ and mitigate the polarization induced by the nonlinear transport of interfacial ions. The modified zinc anode sustains at extreme conditions for over 1573 h (40 mA cm−2, 40 mAh cm−2, DOD = 75.97%) and 490 h (100 mA cm−2, 100 mAh cm−2, DOD = 90.91%), and achieving an unprecedented cumulative capacity of 62.92 Ah cm−2. This work offers both fundamental and practical insights for the interface design in energy storage devices.

This review aims to highlight the effect of electrolyte regulation on alleviating issues on the cathode side in aqueous ZIBs. The recent advances of electrolyte regulation strategies are present, with a comprehensive discussion and summary of regulation mechanisms, which can provide guidance to develop novel and multifunctional electrolytes for next-generation aqueous ZIBs.

Enhancing cathodic performance is crucial for aqueous zinc-ion batteries, with the primary focus of research efforts being the regulation of the intrinsic material structure. Electrolyte regulation is also widely used to improve full-cell performance, whose main optimization mechanisms have been extensively discussed only in regard to the metallic anode. Considering that ionic transport begins in the electrolyte, the modulation of the electrolyte must influence the cathodic performance or even the reaction mechanism. Despite its importance, the discussion of the optimization effects of electrolyte regulation on the cathode has not garnered the attention it deserves. To fill this gap and raise awareness of the importance of electrolyte regulation on cathodic reaction mechanisms, this review comprehensively combs the underlying mechanisms of the electrolyte regulation strategies and classifies the regulation mechanisms into three main categories according to their commonalities for the first time, which are ion effect, solvating effect, and interfacial modulation effect, revealing the missing puzzle piece of the mechanisms of electrolyte regulation in optimizing the cathode.

This study investigates bias-induced structural transformations in 1T-TiSe2 devices, focusing on the transition from the 1T metallic phase to the distorted 1Td phase and ultimately to an orthorhombic Ti9Se2 conducting phase. Using ex-situ and in-situ TEM, dynamic structural changes and insights into the effect of thickness on phase transitions, providing valuable information for CDW-based device applications, are revealed.

Metallic transition metal dichalcogenides (MTMDCs) are of significant attention for various electronic applications due to their anisotropic conductivity, high electron mobility, superconductivity, and charge-density-waves (CDW). Understanding the correlations between electronic properties and structural transformations is crucial. In this study, a bias-induced structural transformation in vertical CDW-based 1T-TiSe2 devices, transitioning from a 1T metallic phase to a distorted transition 1Td phase and subsequently to an orthorhombic Ti9Se2 conducting phase, is reported. Using ex-situ and in-situ biasing transmission electron microscopy, dynamic structural changes, while electron energy loss spectroscopy analysis revealed valence state modifications in Ti and Se within the Ti-rich layer after biasing, are observed. In addition, the effect of varying 1T-TiSe2 thickness on the maximum current value is investigated. These observations reveal that increased thickness requires higher voltage to induce phase transitions. These insights contribute to understanding the structural and electronic dynamics of 1T-TiSe2, highlighting its potential as a promising material for future CDW-based device applications.

Ultra-small silver nanoparticles are formed in situ and activated in an amidoxime-modified polymer of intrinsic microporosity to fabricate a metallic nanocomposite membrane for C2H4/C2H6 separation. The activated silver nanoparticles promote C2H4 transport and effectively enhance C2H4/C2H6 separation selectivity, resulting in an outstanding membrane separation performance with C2H4 permeability of 322.1 barrer and C2H4/C2H6 selectivity as high as 8.8.

The separation of C2H4 and C2H6 is a critical yet energy-intensive operation in the petrochemical industry. Gas separation membranes offer energy-efficient alternatives, but their effectiveness is hindered by the similar physical properties of C2H4 and C2H6. Here, a metallic nanocomposite membrane (MNM) comprising ultra-small Ag nanoparticles embedded in an amidoxime-modified polymer of intrinsic microporosity (AOPIM-1) is reported for highly efficient C2H4/C2H6 separation. The microporous structure of AOPIM-1, combined with anchoring groups (amidoxime groups) inside the microcavities, enables size-controlled growth of Ag nanoparticles with ‒≈3 nm diameter, which maximizes the contact with ethylene molecules. The amidoxime groups as electron acceptors effectively enrich the positive charge on the surface of Ag nanoparticles. The activated Ag form reversible complexes with ethylene molecules endowing them with preferential affinity over ethane. The resulting Ag nanocomposite membrane demonstrates a ≈10-fold increase in C2H4 permeability, reaching 322.1 barrer, and a ≈3-fold increase in C2H4/C2H6 selectivity, reaching 8.8. The comprehensive separation performance is superior over all the polymer membranes and mixed matrix membranes reported so far. The MNMs also demonstrate stable mixed gas separation performance under elevated feed gas pressures. This study provides valuable insights into designing and fabricating polymer membranes with high C2H4/C2H6 separation performance.

A Co single-atom catalyst (Co-N₄) enhances Cl₂ adsorption and lowers LiCl reaction barriers in Li-Cl₂ batteries. The Li-Cl₂@Co-NC battery exhibits >600 cycles at 1500 mA g⁻¹ at room temperature and 650 cycles at 500 mA g⁻¹ at −40 °C, with a 0.6 V reduction in polarization voltage. This strategy delivers high-performance Li-Cl₂ batteries with wide temperature adaptability.

Lithium-chlorine (Li-Cl2) secondary batteries are emerging as promising candidates for high-energy-density power sources and an extensive operational temperature range. However, conventional electrode materials suffer from weak adsorption for chlorine gas (Cl2) and low conversion efficiency of lithium chloride (LiCl), leading to significant loss of chlorine-based active materials. This issue hampers the cyclability of Li-Cl2 batteries. In this work, it is demonstrated that synergistic Cl2 adsorption on the electrode surface and the energy barrier for LiCl reactions are crucial for enhancing Cl2/LiCl conversion efficiency. Consequently, a cobalt (Co) single-atom site catalyst with a Co-N4 coordination environment has been developed, which significantly diminishes the transformation barrier of solid LiCl particles into Cl2 and concurrently enhances the chemical adsorption of Cl2, facilitating uniform nucleation of LiCl. As a result, the Li-Cl2@Co-NC battery developed has achieved a 0.6 V reduction in polarization voltage under high current densities, effectively addressing the issue of low conversion efficiency between Cl2 and LiCl. At room temperature, the Li-Cl2@Co-NC battery achieves over 600 cycles at 1500 mA g−1; At −40 °C, it reaches 650 cycles at 500 mA g−1. The research overcomes the cycle stability barrier in high-current Li-Cl2 batteries and offers a strategy for batteries with a wide temperature range and long cycle life.