Implant-associated infections (IAIs), particularly those caused by antibiotic-resistant pathogens and protected by biofilms, remain a formidable challenge in orthopedic surgery due to limited antibiotic efficacy and sustained local immunosuppression. Addressing this dual bottleneck, we report a multifunctional MoS₂@Fe₃O₄ heterostructure nanocomposite that enables ultrasound (US)-triggered piezocatalytic antibacterial therapy coupled with immune microenvironment remodeling. The nanoplatform integrates the piezoelectric polarization of MoS₂ and the Fenton-like catalytic activity of Fe₃O₄ to achieve efficient charge separation, interfacial polarization, and enhanced Fe³⁺/Fe²⁺ cycling, generating high levels of ROS (•OH, •O₂⁻, ¹O₂) under low-intensity US irradiation. These reactive species effectively disrupt MRSA biofilms, promote bacterial membrane rupture, and expose pathogen-associated antigens. Importantly, this treatment activates the cGAS–STING signaling axis in dendritic cells, enhances M1-type macrophage polarization, and triggers coordinated innate and adaptive immune responses. In a murine subcutaneous IAI model, MoS₂@Fe₃O₄ + US not only eradicated biofilm infections and reduced myeloid-derived suppressor cell (MDSC) infiltration, but also induced robust CD4⁺/CD8⁺ T cell activation and memory B/T cell formation, effectively preventing infection recurrence after implant replacement. This work presents a paradigm-shifting, non-antibiotic immunotherapeutic strategy that integrates catalytic disinfection, immune activation, and long-term protection in a single nanoplatform. By overcoming key limitations of current treatments, our approach offers substantial promise for improving clinical outcomes in IAIs and advancing the field of immune-interactive nanomedicine.

Abstract Liquid crystal elastomers (LCEs) are promising soft actuators, yet their permanently crosslinked networks severely limit end-of-life recyclability. Although dynamic covalent bonds have enabled reprocessability, closed-loop chemical recycling that allows high-yield recovery of reusable molecular building blocks while preserving actuation performance remains challenging. Here, we report a closed-loop chemically recyclable LCE constructed from commercially available reagents via a two-step synthesis. The network is crosslinked by boronic ester bonds formed between a vicinal-diol-bearing liquid crystal oligomer and 1,4-phenylenediboronic acid (PBBA). By varying the PBBA content, the thermal, mechanical, and actuation properties of the LCEs can be systematically tuned. The optimized monodomain LCEs exhibit reversible thermal actuation with good cycling stability. Under mild solvent-assisted hydrolysis conditions, the boronic ester crosslinks are selectively cleaved, while the thioether backbone remains intact, enabling high-yield recovery of both PBBA and the LC oligomer. The recovered components can be directly reconstituted into renewed LCE actuators with thermal, mechanical, and actuation properties closely matching those of the pristine materials. A cascading closed-loop recycling demonstration further shows that the same recovered building blocks can be successively transformed from a 2D film actuator to a 3D tubular actuator and then to a thermally responsive smart surface. This work provides a practical component-level closed-loop recycling strategy for sustainable LCE actuators.

As a new generation of high-energy-density energy storage system, solid-state aluminum-ion batteries have attracted much attention. Nowadays polyethylene oxide (PEO)-based electrolytes have been initially applied to Lithium-ion batteries due to their flexible processing and good interfacial compatibility, their application in aluminum-ion batteries still faces problems. To overcome the limitations in aluminum-ion batteries-specifically, strong Al3+ coordination suppressing ion dissociation, high room-temperature crystallinity, and inadequate mechanical strength-this study develops a blended polymer electrolyte (BPE) of polypropylene carbonate (PPC) and PEO. The PPC disrupts PEO crystallization, creating continuous amorphous channels that boost Al3+ mobility to 0.597 and enhance ionic conductivity. Simultaneously, rigid PPC chains form a dual-network structure with flexible PEO, increasing tensile strength to 672 kPa to effectively suppress aluminum dendrites. Crucially, PPC's carbonyl groups (─C═O) strongly adsorb Al3+ (-1.49 eV), partially displacing PEO's ether-oxygen coordination. This decouples ion pairs, elevates free Al3+ concentration, and improves interfacial kinetics. Consequently, Al//Al symmetric cells achieve stable 200-h cycling (0.1 mA cm-2, overpotential <0.4 V), and Al//benzo[i]benzo[6,7]quinoxalino[2,3,9,10]phenanthrol[4,5-abc]phenazine-5,10,16,21-tetraone (BQPT) cells retained 130 mAh g-1 after 120 cycles at 1 A g-1, demonstrating a promising high-safety electrolyte.

Due to its low cost, high theoretical capacity, and high voltage platform, MnO2 is of significant interest for aqueous aluminum-ion batteries (AAIBs). However, issues such as irreversible phase transitions, manganese dissolution, and low conductivity limit its rate performance and lifespan. This study introduces a hybrid 1.14 % AlxMnO2@g-C3N4 (AMOCN) cathode, combining Gibbs free energy-driven Al3+ pre-insertion with g-C3N4 surface modification. By reinforcing the tunnel structure and repairing surface vacancies, the AMOCN cathode effectively mitigates manganese dissolution. Theoretical calculations indicate that Al3+ pre-intercalation modifies the intrinsic structure of MnO2, enhancing its kinetics. The g-C3N4 coating forms a strong bond with MnO2, reducing the impact of active water on oxygen vacancies and further decreasing Mn2+ dissolution while suppressing the hydrolysis reaction. Electrochemical and ex-situ characterizations reveal the staged insertion behavior of H+ and Al3+ in the MnO2 matrix and a dual-storage mechanism involving MnO2 and g-C3N4. The AMOCN cathode demonstrates improved capacity and stability, maintaining a capacity of 126.23 mAh g- 1 after 300 cycles at 0.5 A g- 1. This work offers new insights for developing robust tunnel structures and optimized interface designs for organic/inorganic hybrid cathodes.

In recent years,aqueous aluminum ion batteries have been widely studied owing to their abundant energy storage and high theoretical capacity.An in-depth study of vanadium oxide materials is necessary to address the precipitation of insoluble products covered cathode surface and the slow reaction kinetics.Therefore,a method using a simple one-step hydrothermal preparation and oxalic acid to regulate oxy-gen vacancies has been reported.A high starting capacity(400 mAh g1)can be achieved by Ov-V2O5,and it is capable of undergoing 200 cycles at 0.4 A g-1,with a termination discharge capacity of 103 mAh g-1.Mechanism analysis demonstrated that metastable structures(AlxV2O5 and HxV2O5)were constructed through the insertion of Al3+/H+during discharging,which existed in the lattice intercalation with V2O5.The incorporation of oxygen vacancies lowers the reaction energy barrier while improving the ion transport efficiency.In addition,the metastable structure allows the electrostatic interaction between Al3+and the main backbone to establish protection and optimize the transport channel.In parallel,this work exploits ex-situ characterization and DFT to obtain a profound insight into the instrumental effect of oxygen vacancies in the construction of metastable structures during in-situ electrochemical activa-tion,with a view to better understanding the mechanism of the synergistic participation of Al3+and H+in the reaction.This work not only reports a method for cathode materials to modulate oxygen vacan-cies,but also lays the foundation for a deeper understanding of the metastable structure of vanadium oxides.

Leveraging anionic redox chemistry (ARR) has emerged as a promising strategy for voltage-dependent capacity enhancement in Zn- and Li-ion batteries. Yet, the realization of such redox activity in aqueous aluminum-ion battery (AAIB) systems, particularly through MnO2-based cathode architectures, remains a critical scientific challenge due to unexplored electrochemical mechanisms under aqueous electrolyte conditions. In this study, a novel MnO2 micro-nanoflower cluster (CaMnO-140) is introduced. The structure, featuring Ca2+ pillars and manganese vacancies (VMn), induces non-bonding O 2p states, activating ARR and facilitating Al3+ storage via three-dimensional diffusion channels. The pre-inserted Ca2+ ions form stable Ca-O bonds with lattice oxygen, suppressing interlayer sliding and Jahn-Teller distortion of Mn(III)Os octahedra, and thereby improving structural stability. Density functional theory calculations elucidate the origin of anionic redox reaction activation and the enhanced ionic transport properties in CaMnO-140. Ex-situ characterizations further confirm reversible oxygen redox processes driven by the uptake and release of CF3SO3- from the electrolyte, along with manganese redox and co-insertion/extraction of H+ and Al3+ ions. This work establishes a paradigm for anion redox-driven material design in AAIBs, bridging the gap between fundamental redox mechanism understanding and practical high-capacity energy storage applications.

Bimetallic oxides (V0.95Mo0.97O5) characterized by easy accessibility, abundant redox reactions, and high capacity are considered promising cathode materials for aqueous aluminum ion batteries (AAIBs). However, their inherent low conductivity and high impedance significantly limit their electrochemical performance. In this work, we enhance the active ion diffusion rate and increase the number of active sites by in situ synthesizing V0.95Mo0.97O5 (VMO) on Mo2V2C3Tx (MVT). The microtoughness of the cathode material is substantially improved by forming bimetallic bonds (Mo-V), which facilitates the reversible intercalation of aluminum ions and induces changes in the (100) crystal surface. The de-insertion mechanism of aluminum ions is elucidated through ex-situ characterization techniques. Furthermore, density functional theory (DFT) calculations validate electrochemical kinetics and stability enhancement in bimetallic oxides facilitated by MVT. This study extends the range of AAIB cathode materials and provides new insights into applying bimetallic solid MXene in aqueous batteries.

Given its high safety standards, the aqueous battery is anticipated to be introduced as the next generation of flexible battery. Nevertheless, issues such as the uncontrollable passivation of the anode, HER and the low toughness of the hydrogel still require resolution. Hydrogen evolution reaction in a conventional liquid electrolyte is unavoidable, and its uncontrolled Al3+ deposition often forms dendritic structures with high surface energy, which quickly reacts with water/oxygen to form an insulating passivation layer. For this purpose, a synergistic hydrogel electrolyte is developed, which provides homogeneous ion-transport channels, displaces water molecules coordinated with Al3+ (a large number of carboxyl groups and hydroxyl groups), and guides them to shuttle quickly and deposit stably in the anode., reduces hydration activity, effectively inhibits hydrolysis, and regulates Al3+ deposition kinetics. Meanwhile, its mechanical properties are further enhanced by the "salting out" action in the Hofmeister effect. The incorporation of SO42-ions enhance the hydrogen bonds of the polymer chains, and the breaking strength exceeds five times that of the original hydrogel without Al2(SO4)3 soaking. As a result, the assembled Al//Al symmetric battery has obvious cycling advantages compared with other aluminum salt-soaked electrolytes. Furthermore, the favorable interface contact between the hydrogel and the electrode ensures that the PTO/Al batteries can still undergo stable cycling when subjected to external forces. This work provides a new way to develop safe and high-performance flexible aluminum batteries.

Vanadium oxide cathode materials in aqueous aluminum‐ion batteries (AAIBs) have an exceptional potential for development because of their high valence and fast electron transfer capability. However, the strong electron–electron Coulomb repulsion in vanadium and its associated electrostatic interactions severely hinder the feasibility of vanadium oxides in AAIBs. The glucose‐assisted hydrothermal reduction of monoclinic VO 2 combined with Cu ion doping effectively promotes the self‐assembly of VO 2 into nanoflower architectures, enabling precise control over morphology and crystalline structure. When integrated with a 5 m Al(OTF) 3 electrolyte and an Ionic liquid （IL ）‐treated Al sheet anode, this full battery demonstrates outstanding electrochemical performance, achieving an initial discharge capacity of 642 mAh·g −1 at 0.4 A·g −1 . Moreover, introducing Cu 3d orbitals effectively enhances the hybridization and electronic coupling effects between the V 3d and O 2p orbitals. Ex situ characterization and diffusion kinetic provide insights into the embedding/de‐embedding mechanism of Al 3+ . This work significantly improves the application potential of VO 2 in AAIBs through structural optimization and mechanism studies and provides systematic scientific guidance for the development of vanadium oxide cathode materials.

Metal-organic frameworks (MOFs) with characteristics of metal ion hosts and organic ligand guests show promising applications in aqueous aluminum ion batteries (AAIBs). However, the sluggish kinetics and poor stability have detrimental effects on their practical application. Herein, an F-doped manganese-based metal-organic framework (Mn-MOF-74) was synthesized via a hydrothermal method. Mn-MOF-74 provides additional redox sites. Due to the high electronegativity of F and the high bond energy of C-F, the F-doping strategy has successfully improved the kinetics and stability. Electrochemical analysis and density functional theory (DFT) calculations jointly demonstrate the activation process of Mn-MOF-74. In addition, the energy storage mechanism has been systematically investigated by ex situ characterization. The organic linker provides additional active sites in which C-O and C-O undergo reversible changes. This work provides not only a feasible way to improve cycling stability but also a deeper understanding of the reaction mechanism related to MOFs in AAIBs.

Molybdenum oxide (MoO3) shows significant potential for use in aqueous aluminum-ion batteries (AAIBs) due to its high theoretical specific capacity and unique layered structure. However, its application is hindered by poor conductivity, volume expansion, and structural instability in aqueous electrolytes, which severely limit its performance in AAIBs. In this study, MoO3 is combined with carbon spheres using a hydrothermal method with pH regulation. The resulting composite significantly enhances the conductivity and structural stability of the electrode, ensuring improved performance during charging and discharging. pH regulation further enhances the adsorption of MoO3 onto the carbon spheres and influences the cathode morphology, increasing both the specific surface area and the active sites. Experimental results show that the composite retains an initial discharge capacity of 195.55 mAh g- 1 and a Coulombic efficiency exceeding 92 % after 140 cycles at a current density of 0.4 A g- 1, demonstrating excellent aluminum storage performance. Additionally, the reaction mechanism of Al3+ insertion and extraction in AAIBs is clarified through ex-situ characterization. This work offers practical solutions to the challenges associated with molybdenum-based oxides in aqueous batteries, facilitating their further development and application in this field.

The shuttle effect of aluminum polysulfides (AlPSs) have been a source of concern for studying Al/S batteries. Due to the weak adsorption of C-S composites, research on cathode materials for Al/S batteries has been delayed. As it is generally known that Al2S3 decomposition demands a large Gibbs free energy, this work has tried to reduce the Al2S3 decomposition potential energy. Herein, the Ni/Co bimetallic selenide reduces the energy barrier conversion and mitigates the polarization effects, while morphology control enables the storage and anchoring of S, alleviating the shuttle effect. Additionally, the intermediate products serve as single-atom catalysts, increasing the active sites, synergistically enhancing the ion diffusion kinetics. DFT calculations verify that NiCo2Se4 has a moderate Gibbs free energy change during the rate-limiting step of S reduction and the most robust adsorption energy to Al2S3. NiCo2Se4@CS2/Al has a remaining capacity of 135 mAh/g after 450 cycles (at 200 mA g(-1)), pioneering novel ideas for the development of Al/S batteries.

Aqueous aluminum ion batteries (AAIBs) have garnered extensive attention due to their environmental friendliness, high theoretical capacity, and low cost. However, the sluggish reaction kinetics and severe structural collapse of the cathode material, especially manganese oxide, during the cycling process have hindered its further application. Herein, Cu2+ pre-intercalated layered δ-MnO2 was synthesized via a hydrothermal method. The pre-intercalated Cu2+ ions not only improve the conductivity of MnO2 cathode but also stabilize the structure to enhance stability. X-ray absorption fine structure (XAFS) combined with density functional theory (DFT) calculations confirm the formation of the covalent bond between Cu and O, increasing the electronegativity of O atoms and enhancing the H+ adsorption energy. Moreover, ex-situ measurements not only elucidate the Al3+/H+ co-insertion energy storage mechanism but also demonstrate the high reversibility of the Cu-MnO2 cathode during cycling. This work provides a promising modification approach for the application of manganese oxides in AAIBs.

Liquid crystal elastomers (LCEs) are versatile soft actuators known for their flexible texture, low density, and ability to undergo reversible deformations that mimic the behavior of skeletal muscles. These properties make them highly attractive for applications in exoskeletons, soft robotics, and medical devices. However, their functionality is typically limited to simple and discontinuous deformations. This study introduces a novel structural design that enables precise control of both the mode and amplitude of deformation. This design integrates photo-reactive o-nitrobenzyl moieties and temperature-dependent hydrogen bonds into the LCE structure. The o-nitrobenzyl moieties enable irreversible reconfiguration of the LCE crosslinked network through photoreactions, allowing for easy alignment and reshaping of the material. Meanwhile, the hydrogen bonds act as "temperature-dependent locks", regulating the mobility of polymer chains during thermal deformation. By adjusting the heating temperature, the deformation amplitude can be finely tuned across a wide range (0%-103%). The synergy of these two mechanisms-light-induced irreversible reconfiguration and temperature-induced reversible H-bond exchanges-empowers LCEs to achieve customizable and continuous deformations. This represents a significant advancement in bridging the gap between synthetic actuators and biological motion systems.

Metal aluminum is inexpensive, pollution-free, safe to use, and abundant in resources. It has great potential in electrochemical energy storage, with a theoretical specific capacity of up to 2980 mAh g(-1). Sulfur not only has the advantages of abundant raw materials and low prices, but also has a theoretical capacity of 1675 mAh g(-1). The theoretical energy density of Al-S batteries can reach up to 1340 Wh kg(-1) when matched with metallic aluminum. However, the current research on Al-S batteries is still in its early stages, and the impact of differences in electrolyte systems on the electrochemical performance and working mechanism of Al-S batteries is not yet clear. The research on the electrochemical reaction mechanism, capacity degradation mechanism, and strategies to improve charge transfer kinetics of aluminum sulfur batteries is crucial for improving their electrochemical performance. From this perspective, this paper comprehensively summarizes the electrochemical performance, charging/discharging mechanisms, and battery level cost advantages of Al-S batteries with different electrolyte systems. The influence of the phase transition process of S and the shuttle effect of polysulfides on the electrochemical performance of Al-S batteries is elucidated based on different electrolyte systems. In addition, in response to the key issues currently existing in Al-S batteries, the next research directions are summarized and prospected.

Aqueous aluminium ion batteries (AAIBs) have attracted much attention due to their high theoretical capacity, safety, and environmental friendliness. However, the Research and Development (R&D) of cathode materials has limited its development and application. MoO3 has been proven to be a reliable and stable cathode material, nevertheless, it faces the dilemma of poor cycling performance and low specific capacity in AAIBs due to the irreversible phase transition in its structure. In this paper, MoO3 synthesized by a hydrothermal method has a unique nanobelt structure, which significantly enhances the structural stability of MoO3 and reduces its structural damage during charging/discharging. In addition, the nanobelt structure also gives MoO3 a rougher surface, which provides a large number of active sites and spaces for the insertion and extraction of Al3+ and improves the diffusion rate of Al3+ to a large extent. Experimental results demonstrate that this MoO3 nanobelt cathode exhibits significantly improved cycling stability and high specific capacity in AAIBs. This paper provides a practical solution to the existing challenges of AAIBs and further promotes the development and application of molybdenum-based materials in AAIBs.

Organic cathodes have gained increasing attention in the field of aqueous batteries due to their molecular design flexibility and environmental friendliness. Among them, n-type organic compounds are favored for their unique ionic coordination mechanism and high capacity due to multiple active centers. Herein, an organic material, Diphenazino[2,3-b](5,6,12,13-tetrahydropyrazino[2',3':9,10]phenanthro[4,5-fgh]quinoxaline) (DTPQ) enriched with multiple C═N groups is designed by hot solvent condensation as rechargeable aqueous aluminum batteries (AABs) cathodes. The enriched imine group as active centers provides good specific capacity and capacity retention and exhibits excellent reaction kinetics. The extension of the π-conjugated structure also enables DTPQ to exhibit excellent rate capability while ensuring structural stability. In addition, theoretical calculations confirm the improvement of ion storage redox kinetics by the π-conjugate extension brought about by the rich electronic states and high aromatic backbone. Meanwhile, the storage mechanism of the imine group for Al-containing cations is explained by a series of ex situ characterizations. New ideas are provided for the design and application of n-type organic cathodes in AABs.

Liquid crystal elastomers (LCEs) are important soft actuators that show strong promise in many fields where traditional rigid actuators or robotics are impractical. However, their real-world applications are lacking primarily due to inadequate actuation performance and complicated fabrication processes. Here, a novel design is reported that significantly enhances actuation performance while simplifying the fabrication process. The design involves constructing densely entangled structures by synthesizing high-molecular-weight linear LCEs (>180 kDa) with a moderate number of side groups in a single step. These entangled structures greatly enhance mechanical strength while maintaining toughness, resulting in an ultra-high actuation work capacity (1427 kJ m- 3). By applying melt shearing or solvent treatment, these entanglements can be temporarily disrupted, providing thermoplastic-like processability. With these properties, lightweight wearable devices (<10 g) capable of generating over 30 N of contractile force are developed, which is sufficient to reversibly lift an adult male's arm. This work employs a single fabrication step to develop densely entangled LCEs with exceptional actuation performance and thermoplastic-like processability, signaling a bright future for their applications in rehabilitation devices, wearables, and beyond.

Liquid crystal elastomers (LCEs) are promising soft actuators, yet conventional covalently crosslinked systems typically suffer from limited reprocessability and reprogrammability. Here, supramolecular LCEs (SLCEs) are reported that incorporate acylsemicarbazide (ASC) moieties as dynamic hydrogen-bonded crosslinks within a linear polyurethane-urea backbone. Using a simple two-step polymerization, hydrogen bond density and strength are systematically modulated by varying the hard-segment content (18.3-26.9 wt.%) and ASC chain-extender structure, respectively, resulting in SLCEs with tunable thermal, mechanical, and actuation responses. The maximum work capacity reaches 260 kJ m(-)(3), more than twice that of previously reported hydrogen-bonded SLCEs, and replacing an aliphatic dihydrazide chain extender with terephthalic dihydrazide yields an actuation strain of 72%, among the highest reported for SLCEs. The dynamic network also enables scalable fabrication of actuators with programmable deformation through melt extrusion and injection molding at moderate temperatures (<120 degrees C). In addition, these materials demonstrate robust self-healing and recyclability. This generalizable molecular design combines high actuation performance with thermoplastic-like processability, opening opportunities for sustainable, reprocessable soft actuators.

A humidity-responsive blue phase liquid crystal polymer film (alkalized-acrylic-BP) based on an interpenetrating polymer system has been fabricated.