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4D printing has attracted widespread attention due to its ability to fabricate complex structures capable of responding to specific stimuli. However, existing smart materials used for 4D printing, such as conventional hydrogels, liquid crystal elastomers, and shape‐memory polymers, are constrained in their ability to fulfill both mechanical ultrastrength and ultrastretchability requirements simultaneously due to their water saturation or uneven network structures. This study presents 4D printing of liquid‐free ionic elastomers (LFIEs) that is achieved through photopolymerization of the acrylic acid‐tetramethylammonium chloride‐polymerizable deep eutectic solvent. The transition temperature (Tt) of the high‐fracture‐strength LFIEs is adjusted by introducing phenylphosphoric acid, harboring multiple hydrogen‐bonds, leading to improved molecular chain mobility through softening of the chains. Consequently, the 4D‐printed LFIEs retain their high strength while achieving ultrastretchable properties even under elevated temperatures during heating. Moreover, the 4D‐printed LFIEs demonstrate both a swift response time and a high fixation rate even after undergoing repeated transformation cycles. These outstanding capabilities exhibit by LFIEs present a reliable strategy for advancing their applications in diverse fields, such as smart furniture, robotics, and intelligent manufacturing with remote monitoring, and beyond. [ABSTRACT FROM AUTHOR]

Battery recycling is a promising approach to mitigate the safety, environmental, and economic threats posed by numerous discarded lithium‐ion batteries (LIBs). However, the unclear atomic‐scale degradation of spent graphite complicates recycling, resulting in energy‐intensive impurity removal and graphitization, which hampers industrialization. This study uses Cryo‐transmission electron microscopy (Cryo‐TEM) to characterize spent graphite degradation and develop a scalable graphite self‐induced microwave plasma method for efficient regeneration. Cryo‐TEM images show graphite coated with a solid electrolyte interphase (SEI) layer, revealing lattice defects and structure expansion near the surface that impair electrochemical performance. The self‐induced microwave plasma method eradicates the SEI layer and restores the graphite lattice structure within 30 s. Multiphysics simulations indicate that the microwave field generates a strong electric field on the graphite surface, causing plasma discharge and rapid surface heating. Regenerated graphite demonstrates excellent electrochemical performance, with a specific charge capacity of 352.2 mAh g−1 at 0.2 C and ≈81% capacity retention after 400 cycles, matching commercially available materials. This efficient method offers a promising approach for recycling graphite anodes. [ABSTRACT FROM AUTHOR]

Miniature soft actuators have garnered attention across healthcare, military, and industrial fields; however, soft actuators mostly have functions and applications in nature‐inspired biomimetic locomotion, without any specific approaches reported for biomedical applications. In biomedical applications, soft actuators must be biodegradable, biocompatible, and visible in vivo. This study presents a multifunctional soft actuator comprising chitosan and magnetic nanoparticles (MNPs) fabricated via facile casting and laser micromachining. The actuator demonstrates programmable shape morphing and responds swiftly to six stimuli: humidity, chemical solvents, near‐infrared (NIR) light, radio‐frequency (RF) heating, temperature, and magnetic fields. This actuator shows feasibility for biomimetic applications, such as flower, leaf, larva, and finger. Furthermore, the actuator demonstrates magnetic locomotion, real‐time X‐ray visibility, biocompatibility, and biodegradability both in vitro and in vivo. The multistimulus‐responsive shape‐morphing performance of the soft actuator has potential as a wireless miniature robot in various fields, including biomimetic and biomedical applications. [ABSTRACT FROM AUTHOR]

Transition metal carbides (TMCs) grown by chemical vapor deposition (CVD) offer promise for numerous novel phenomena and applications in the 2D limit. Despite considerable efforts thus far, the flexible customization of TMCs and their heterostructures still remains challenging. Herein, a substrate engineering is developed to achieve customized manufacturing of ultrathin WC single crystals and WC/graphene (WC‐G) heterostructures by varying the concentration of Zn in Cu‐Zn alloy substrate. It is worth noting that Zn atoms can remarkably reduce the nucleation density of graphene and promote the nucleation of WC. Thus, an increasing Zn content is applied to synergistically modulate the growth of graphene and WC, enabling the controllable fabrication of WC and WC‐G heterostructures. The synthesized WC crystals exhibit an ultrathin nature down to 3 nm, as well as high crystalline, ultra‐clean surface, and superb chemical stability. Based on that, the typical metallic properties with a temperature‐dependent resistance (nearly 1.30 Ω at 300 K and nearly 0.08 Ω at 1.7 K) and low resistance as well as excellent nonlinear optical performance of WC are demonstrated. This work provides fresh insights into regulating the growth behavior of multiblock‐structured carbides and promotes the study of their optic and electronic properties. [ABSTRACT FROM AUTHOR]

The nickel‐iron based materials are widely studied as excellent oxygen evolution reaction (OER) electrocatalysts. However, its relatively poor OER stability limits its practical applications. Herein, a zipper‐like interlocked heterostructure of NiFe layered double hydroxide (LDH)‐WN is constructed. The NiFe LDH‐WN exhibits not only ultrahigh OER activity of 228 mV overpotential at a current density of 50 mA cm−2, but also extremely long‐term stability over 4500 h at 50 mA cm−2 and over 550 h at an industrial current density ≈350 mA cm−2, which is ascribed to its special zipper‐like interlocked structure. Moreover, in situ Raman confirms that the presence of WN can efficiently achieve NiFe LDH reconstruction to slower the metal dissolution during OER, and therefore boosts its stability. DFT calculations reveal that WN not only can increase the *O adsorption capability and conductivity of NiFe LDH layer, but also can anchor the metal atoms of NiFe LDH layer to improve the dissolution energy barrier. In short, this work presents a new method of constructing the interlocked heterostructure to improve the OER stability of Ni‐Fe‐based catalysts, which would accelerate its practical application. [ABSTRACT FROM AUTHOR]

Establishing a reliable control of perpendicular magnetic anisotropy (PMA) is challenging but essential for the full utilization of rare‐earth iron garnets in spintronic devices. In this study, a feasible approach to enhance the PMA of ferrimagnetic thulium iron garnet (TmIG) films is presented. This approach involves precise adjustments in cation stoichiometry and epitaxial strain state. By fine‐tuning the pre‐ablation process and oxygen partial pressure during pulsed laser deposition, a series of high‐quality TmIG films can grow with variable cation stoichiometry, i.e., the Tm/Fe molar ratio. The finding reveals that cation stoichiometry plays a crucial role in determining the magnetic properties of the TmIG films. Particularly, the stoichiometric TmIG film has the strongest PMA due to the maximized magnetostriction coefficient. Combining this stoichiometry optimization and strain engineering, an unprecedented PMA strength of ≈30 kJ m−3 for TmIG is achieved. This achievement demonstrates a simple and effective method for harnessing the magnetic properties of rare‐earth iron garnet films, paving the way for their advanced applications in next‐generation spintronic devices. [ABSTRACT FROM AUTHOR]

Electrochemical CO2 reduction reaction (CO2RR) provides a promising way for producing value‐added fuels and chemicals via renewable electricity. However, the dynamic reconstruction of electrocatalysts of atomic active sites hinders in‐depth understanding of catalytic mechanism and further industrial application, especially under ampere‐level current density conditions. In this work, electro‐induced crystallization is reported over an amorphous Indium hydroxide gel (In gel) catalyst, which generates active sites for efficient and selective CO2RR. Molecular dynamic calculation reveals the crystallization process can maintain amorphous In‐OH species on the surface while generating crystallized metallic In under electroreduction condition; structural characterizations prove that the derived partially crystallized In gel is stable consisting of amorphous/crystalline interface, even biased at a high polarization potential of −4 V versus reversible hydrogen electrode. The resultant partially crystalized In gel exhibits a highly selective CO2RR performance toward formate under an ampere‐level current density up to 1200 mA cm−2 simultaneously with 91.89% Faradaic efficiency, which can motivate a high formate generation rate of 20.55 mmol h−1 cm−2. The operando Raman spectroscopic and density functional theoretic results demonstrate the optimized adsorption of *HCOO intermediate for the enhanced formate activity and selectivity over the partially crystallized In gel. [ABSTRACT FROM AUTHOR]

Aqueous Zn-metal batteries are considered promising candidates for next-generation energy storage. However, low zinc utilization rate (ZUR) and limited cycle life are still hinder its commercial application because of severe parasitic side effects. Herein, inspired by the wound healing process, an innovative electrode recovery technology is developed to improve the comprehensive ZUR and prolong the cycling life through repetitive rejuvenation of zinc anode by designing chitosan-based homologous gel/solid synergistic electrolyte. The designed synergistic electrolyte, consisting of protonated chitosan gel electrolyte and Zn-chitosan solid electrolyte, exhibits superior zinc ion diffusion capability and low free-water activity, leading to dendrite-free Zn deposition and HER inhibition. Moreover, through proton neutralization and zinc ion complexation, the formulated electrolyte can implement the rejuvenation of zinc anode by smoothing interfacial defects and eliminating parasitic byproducts. Consequently, the gel/solid synergistic electrolyte displays reversible Zn plating/stripping chemistry for 4000 cycles with high average Coulombic efficiency (99.8%) and realizes comprehensive ZUR of 97.4% through four iterations of electrode recover under extreme conditions (20 mA cm[sup -2], 31.5% Zn depth of discharge), noticeably higher than zinc electrode with no recover (11.8%). Furthermore, the superiority of customized synergistic electrolyte is further demonstrated by coupling with I[sub 2] cathode and achieving impressive 36 000 stable cycles. [ABSTRACT FROM AUTHOR]

Aqueous Zn metal batteries hold significant promise for large‐scale energy storage owing to their high safety and low cost. Nevertheless, severe corrosion and uncontrollable dendrite growth hinder the cyclic stability of Zn metal anodes. Herein, a porphyrin‐Zn(II) (ZnTBPP) based multifunctional artificial layer to stabilize Zn anodes by suppression of hydrogen evolution reactions is designed. This hydrophobic interfacial layer repels active water molecules and facilitates the electron transfer from Zn interface to the ZnTBPP layer, thereby increasing the inherent hydrogen evolution potential of Zn anodes. Differential charge density maps reveal that the electron cloud density of the charge transfer layer within the ZnTBPP layer is delocalized due to the electron‐withdrawing effect of Br‐containing functional groups in the ZnTBPP ligands, depleting the interfacial electrons of Zn metal anodes. As a result, H* exhibits a higher Gibbs free energy (∆GH*) of 0.75 eV on Zn with a ZnTBPP coating layer in contrast to bare Zn (0.55 eV), effectively suppressing H2 production. Specifically, the H2 evolution rate of ZnTBPP@Zn (4.06 µmol h−1 cm−2) is ≈2.2 times lower than that of bare Zn. The ZnTBPP@Zn//NaV3O8·1.5H2O full cells exhibit an ultra‐long cycling life of 10 000 cycles at 10 A g−1. [ABSTRACT FROM AUTHOR]

Aqueous zinc–iodine (Zn–I2) batteries, with their outstanding merits in safety, cost, and environmental friendliness, have received extensive attention. However, the unstable electrochemistry at the electrode–electrolyte interface originating from free water results in zinc dendrite growth, hydrogen evolution reaction (HER), and polyiodide ions shuttle, hindering their practical applications. Herein, solid‐state Zn–I2 batteries based on an inorganic ZnPS3 (ZPS) electrolyte are developed to overcome inherent interfacial issues associated with aqueous electrolytes. The inorganic ZnPS3 electrolyte, with a low Zn2+ diffusion energy barrier of ≈0.3 eV, demonstrates an exceptional ion conductivity of 2.0 × 10−3 S cm−1 (30 °C), which also satisfies high chemical/electrochemical stability and mechanical strength. The solid Zn2+ conduction mechanism, facilitated by bounded water only on grains, effectively suppresses HER and polyiodide ions shuttling. During cycling, a ZnS functional layer is spontaneously formed on the anode/electrolyte interphase, promoting dendrite‐free Zn deposition behavior with a more stable (002) crystal orientation. Consequently, the solid‐state configuration of Zn–I2 battery enables an impressive reversible capacity of 154.2 mAh g−1 after 400 cycles at 0.1 A g−1. Importantly, the compatibility of the solid‐state ZnPS3 electrolyte is also confirmed in the Zn||CuS cell, indicating its potential as a versatile platform for developing inorganic solid‐state zinc‐ion batteries (ZIBs). [ABSTRACT FROM AUTHOR]

Although the electrochemical properties of various cathode candidates for sodium‐ion batteries (SIBs) are intensively studied on the material level, the evaluation and comparison from the perspective of future practical implementation are still lacking. In particular, air stability, which is often overlooked, will not only affect the electrode manufacturing processes but also cause detrimental structural change. Herein, two recently commercialized cathode products of NaNi1/3Fe1/3Mn1/3O2 (NFM) and Na3V2(PO4)3 (NVP) are adopted to evaluate their stability in ambient atmospheres and investigate the structural degradation mechanisms. Theoretical calculations and experimental results demonstrate that the stability of NFM is significantly inferior to that of NVP during air exposure owing to the thermodynamically preferred chemical transformation of NFM. Furthermore, Raman mapping and X‐ray diffraction (XRD) measurements reveal the generation of alkaline, which accelerates the structural degradation of NFM. Accordingly, a simple second‐sintering strategy is proposed to enhance the air stability of NFM by removing impurities and retrieving surface‐precipitated Na+ into the crystalline host. In situ XRD reveals the stabilized crystal structure after the second‐sintering treatment not only effectively inhibits the chemical transformation of NFM in air but also endows the improved cycling stability (a high capacity retention of 90.7% after 200 cycles). [ABSTRACT FROM AUTHOR]

Developing low‐cost and high‐efficient bifunctional catalysts for hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) is greatly significant for water electrolysis. Here, Ni3N‐CeO2/NF heterostructure is synthesized on the nickel foam, and it exhibits excellent HER and OER performance. As a result, the water electrolyzer based on Ni3N‐CeO2/NF bifunctional catalyst only needs 1.515 V@10 mA cm−2, significantly better than that of Pt/C||IrO2 catalysts. In situ characterizations unveil that CeO2 plays completely different roles in HER and OER processes. In situ infrared spectroscopy and density functional theory calculations indicate that the introduction of CeO2 can optimizes the structure of interface water, and the synergistic effect of Ni3N and CeO2 improve the HER activity significantly, while the in situ Raman spectra reveal that CeO2 accelerates the reconstruction of OV (oxygen vacancy)‐rich NiOOH for boosting OER. This study clearly unlocks the different catalytic mechanisms of CeO2 for boosting the HER and OER activity of Ni3N for water splitting, which provides the useful guidance for designing the high‐performance bifunctional catalysts for water splitting. [ABSTRACT FROM AUTHOR]

Atherosclerosis can form intimal plaques in the arteries and undergo plaque rupture with followed stroke or myocardial infarction under certain pathological conditions. However, suboptimal intraplaque accumulation, along with severe off‐target effects, remain formidable obstacles for efficient pharmacotherapy of atherosclerosis. A characteristic feature of the progression of atherosclerosis is the continuous recruitment of inflammatory monocytes that differentiate into foamy macrophages with the generation of legumain in the plaques. In this study, a bio‐activatable nano‐shuttle based on human serum albumin is conceived that contained curcumin to allow the precise inhibition of atherosclerosis progression. Following intravenous injection, the nano‐shuttles are almost exclusively engulfed by inflammatory monocytes in an efferocytosis‐mimetic manner and selectively co‐migrated with the monocytes towards the plaques. The nano‐shuttles are readily activated to release the initially arrested curcumin in response to the generation of legumain upon the differentiation of monocytes into foamy macrophages within the plaques. Treatment assessments on atheroprone apolipoprotein‐E‐deficient mice indicated that the nano‐shuttles substantially inhibit the progression of atherosclerosis by attenuating the plaque inflammation burden without any obvious adverse effects. The integration of highly selective accumulation and specific drug activation of the nano‐shuttles in plaques can arouse an advanced therapeutic strategy to prevent atherosclerotic cardiovascular disease. [ABSTRACT FROM AUTHOR]

Artificial sensory nerves can simulate the functions of visual perception and information processing of the human brain, which is indispensable for the immediate visualization of the environment and awareness requisite to avoid the potential harm. However, it still remains a long‐standing challenge to integrate recognition learning with real‐time processing function in a single device. Herein, an interface defects‐tuning strategy is proposed for developing a novel bi‐functional phototransistor. Benefiting from the tuned polymer‐perovskite layer‐heterointerface defects, the photogenerated charge trapping and de‐trapping capacities are significantly improved, thereby facilitating the photogenerated carrier separation and injection. The prepared organic‐inorganic hybrid phototransistors can perfectly mimic the human visual synaptic behaviors with a quick response speed (<35 ms, far below that of human eyes to incident light (225 ms)). More importantly, the phototransistor exhibited obvious visual adaptation toward wide‐ranging light stimuli, and realized unique desensitization to simulate the self‐protection behavior of the human visual systems. Specifically, the adaptation timescales of the device under dim and high light conditions are superior to bio‐systems (<2 min). Consequently, the reported strategy for the preparation of bi‐functional phototransistors provides a brand‐new perspective for next‐generation artificial nervous systems. [ABSTRACT FROM AUTHOR]

Renal clearance is critical for nanodrug to avoid the long‐term body retention‐related side effects, while it is difficult to achieve efficient tumor accumulation and retention. The over‐developed lysosomes in cancer cells have become an emerging target for more precise and effective cancer therapy. Herein, a pH‐responsive reversible self‐assembled Cu2‐xSe‐BSA, which can be renal cleared under neutral or basic conditions, is developed for selectively targeted aggregation in cancer lysosomes with enhanced tumor accumulation and retention. Moreover, the aggregation of Cu2‐xSe‐BSA can enhance the photoacoustic imaging signal, photothermal therapy, and chemodynamic therapy capability. Cu2‐xSe‐BSA accumulated in lysosomes cannot only induce lysosomes swelling, but also generate reactive oxygen species in situ, causing lysosomal membrane permeabilization and finally lysosomal cell death. Notably, the assembled Cu2‐xSe‐BSA can dissociate to be renal clearable after the treatments are completed and left the acid tumor microenvironment, being of great significance both in scientific research and clinical trial. [ABSTRACT FROM AUTHOR]