The practical applications of lithium-sulfur (Li─S) batteries are impeded by sluggish conversion kinetics of lithium polysulfides (LiPSs) and uncontrolled Li dendrite growth. While introducing single-atom catalysts (SACs) stands out as a promising strategy to overcome these issues, the p-block SACs exhibit great potential. However, the relationship between their synergistic regulation and atomic structure remains unclear. Here, by leveraging the p-electron delocalization induced by the p-π conjugated effect, p-block Se SACs were proposed to synergistically regulate the lithium/sulfur electrochemistry. The experimental and theoretical results demonstrate that the unique Se-C2 coordination structure of Se SACs leads to activated p-electrons, which not only facilitates LiPSs conversion by p-p hybridization but also generates a uniform current distribution to guide Li plating and stripping behavior. Consequently, the Li─S batteries assembled with Se SACs demonstrate a low capacity decay rate of 0.056% per cycle over 1000 cycles at 1 C and achieve a high areal capacity of 5.58 mAh cm-2 under a high sulfur loading of 6.41 mg cm-2 and a low electrolyte/sulfur ratio of 8.3 µL mg-1. This work elucidates the synergistic regulation of Se SACs from atomic orbital level and enlightens the application of p-block SACs in Li─S batteries.

Internal stress control is critical for the electroforming of high-precision components such as X-ray focusing mirrors, which typically require stress levels below 0.1 MPa to maintain shape accuracy. Meanwhile, the complex nonlinear interactions among multiple deposition parameters make stress optimization challenging using traditional methods. We propose a machine learning-assisted framework to systematically investigate and optimize the low-stress (< 0.1 MPa) electroforming of nickel and nickel-cobalt alloys from sulfamate baths. Among various machine learning algorithms, random forest is identified as the optimal predictive model. Based on this, a processing map correlating current density and cobalt concentration with low-stress conditions is established. SHAP analysis reveals that current density is the dominant factor, followed by cobalt concentration. Combined EBSD, XRD, and DFT calculations elucidate the underlying physical mechanisms. Current density induces grain refinement, while cobalt incorporation promotes solid solution formation, both of which lead to lattice expansion in the nickel structure and consequent tensile stress generation. Finally, finite element simulations guide the optimization of engineering solutions, leading to the successful fabrication of X-ray focusing mirrors with exceptional thickness uniformity (coefficient of variation < 2%)

ABSTRACT Layered oxides are promising cathode candidates for sodium‐ion batteries (SIBs) owing to their tunable compositions and high specific capacities. However, detrimental phase transitions, Jahn–Teller (J–T) distortion, and transition‐metal (TM) migration during cycling typically induce severe structural degradation and irreversible oxygen loss, ultimately resulting in rapid capacity fading. Herein, we propose a dual‐scale interlayer‐intralayer synergistic strategy to address these intrinsic challenges, which integrates a P2/O3 biphasic intergrowth architecture for interlayer stabilization and a fence‐type superstructure with enlarged superlattice spacing for intralayer regulation within TM slabs. The intergrown P2/O3 phases generate a robust interlocking effect that alleviates strain accumulation, further suppressing undesirable phase evolution, mitigating J–T distortion, and partially restraining out‐of‐plane TM migration. Meanwhile, the fence‐type superstructure, featuring an ultra‐wide interplanar spacing, inhibits the formation of vacancy clustering driven by in‐plane TM migration, thereby stabilizing the local oxygen environment and eliminating irreversible oxygen loss. Benefiting from this cooperative interlayer‐intralayer regulation, the as‐designed Na 0.668 Li 0.1 Ni 0.3 Mn 0.4 Ti 0.2 O 2 cathode delivers quasi‐solid‐solution reaction behavior and highly reversible oxygen redox, along with substantially enhanced structural stability and electrochemical performance. This work highlights the critical role of dual‐scale structural engineering in simultaneously modulating hierarchical structural motifs, providing a generalizable paradigm for the rational design of high‐energy‐density layered cathodes for SIBs.

In this work, zucchini biochar (ZHB750, ZHB850 and ZHB950) were prepared by freeze-drying and carbonization at different pyrolysis temperatures using widely sourced zucchini (ZH) as raw material. The specific surface area of ZHB950 is 91.466 m2/g, which is 1777

Conjugated polymers have garnered significant attention as promising organic anode materials for sodium-ion batteries (SIBs) due to their tunable chemical structures, high porosity, environmental friendliness, and costeffectiveness. However, inherent limitations of organic electrodes, such as low conductivity, high solubility in electrolytes, and restricted material utilization, hinder their further advancement. Herein, a three-dimensional (3D) porous polyimide (PND) anode material is successfully synthesized via solvothermal polycondensation, with 1,4,5,8-naphthalenetetracarboxylic dianhydride (NTCDA) and 2,6-diaminoanthraquinone (DAAQ) serving as the comonomers. The PND material retains a reversible capacity of 156.1 mAh g-1 with a decay rate of 0.056% per cycle after 1000 cycles at 1.0 A g-1, demonstrating excellent structural stability. The experimental and theoretical results jointly indicate that sodium storage in PND is primarily achieved through reversible enolization of conjugated carbonyl groups, with a notable pseudocapacitive contribution and a Na+ diffusion coefficient reaching 10-9-10-8 cm2 s-1, all of which are closely related to the favorable kinetics enabled by the 3D porous structure. This work offers a novel design strategy for developing high-performance organic electrode materials in SIBs.

Due to their high specific capacity and structural tunability, polyimide (PI)-based organic materials have garnered significant attention for the anode in sodium-ion batteries (SIBs). However, their inherently low electrical conductivity and sluggish interfacial transport kinetics severely constrain electrochemical performance. Herein, this study proposes a dimensional engineering strategy, which involves compositing of carbon quantum dots (CQDs) or multi-walled carbon nanotubes (MWCNTs) with two PI derivatives (PPD and PND). Specifically, one-dimensional MWCNTs facilitate three-dimensional conductive networks that suppress PI stacking and enhance reaction kinetics, whereas zero-dimensional CQDs induce pore blockage. Among all the composites investigated, the PPD doped with 0.1 wt% MWCNTs (PPD@MWCNTs0.1) exhibits the most outstanding electrochemical performance. It delivers a reversible capacity of 166.1 mAh g−1 after 2000 cycles at 1.0 A g−1, maintains sustained stability for over 10000 cycles at 2.0 A g−1, and demonstrates encouraging stability over 50 cycles across a wide temperature range of −30 °C to 60 °C. The pseudocapacitive-diffusion synergy and fast Na+ diffusion coefficient accounts for the exceptional electrochemical performance. In full-cell tests with a NaNi0.5Fe0.5MnO4 cathode, PPD@MWCNTs0.1 delivers stable cycling over 1000 cycles. This work provides a theoretical basis for the development of high-power and durable organic SIBs.

Sodium-ion batteries (SIBs) are emerging as a resource-secure and cost-effective alternative to lithium-ion technologies, owing to the near-limitless abundance of sodium reserves in seawater and terrestrial salt deposits. However, the commercial viability of SIBs remains hindered by the lack of cathode materials that combine high capacity with long-term cycling stability. Herein, we report the rational design and synthesis of a novel chlorine-substituted hexaazatrinaphthylene (HATN-3Cl), exhibiting a rigid, coplanar pi-conjugated framework with six redox-active nitrogen sites. When paired with metallic sodium, HATN-3Cl delivers a reversible discharge capacity of 159 mAh g- 1 after 500 cycles at a current density of 0.05 A g- 1, demonstrating excellent cycling stability and promising application potential. Remarkably, a capacity of 119 mAh g- 1 is retained after 1000 cycles at 1 A g- 1 with an average Coulombic efficiency (CE) of 99.6 %. Galvanostatic intermittent titration technique (GITT) reveals Na+ diffusion coefficients ranging from 10- 8 to 10- 10 cm2 s- 1, attesting to rapid ion transport with minimal activation barriers. Density functional theory (DFT) calculations, corroborated by in-situ Fourier transform infrared spectrometer (FT-IR) and ex-situ X-ray photoelectron spectroscopy (XPS), confirm a highly reversible six-electron redox mechanism proceeding via two-stage Na+ ions insertion at the nitrogen sites. Moreover, the HATN-3Cl electrode sustains its capacity retention and structural integrity across a wide temperature window from -30 degrees C to 60 degrees C, satisfying the operational demands of grid-storage energy storage under extreme climates. This study therefore delivers a scalable, purely organic cathode that bridges the performance gap of SIBs and charts a sustainable pathway toward terawatt-hour-scale energy storage.

The large-scale commercialization of sodium batteries has intensified the need to replace flammable organic electrolytes with solid-state electrolytes (SSEs) to ensure intrinsic safety. This is a key step toward next-generation high performance solid-state sodium batteries (SSSBs). Recently, as a class of crystalline inorganic-organic hybrid materials, metal organic frameworks (MOFs) have been widely used in the frontier research of manufacturing high performance SSEs due to their rich porosity, controllable functionality and modularity. On the one hand, MOFs provide multiple possibilities for regulating the structure-activity connection and electrochemical properties of SSEs. On the other hand, MOFs offer an ideal platform for studying the potential mechanisms of ion conduction and the structure-performance relationship. In this review, the development of recent MOFs-based SSEs for sodium batteries are overviewed, including neat MOFs, ionic liquids (ILs)-laden MOFs, and MOFs incorporated polymer hybrids. For each system, an overview of the advantages was presented, with a discussion of existing and potential challenges and representative design strategies. Additionally, some outlooks for MOFs-based SSEs as the future development directions are provided.

Lithium-sulfur (Li-S) batteries hold great promise for high-energy-density energy storage applications but are plagued by the severe shuttle effect and sluggish conversion kinetics of lithium polysulfides (LiPSs). We herein report a d-p-f orbital coupling strategy to tackle these critical challenges by incorporating Eu 4f orbitals to activate both metallic (Ni) and non-metallic (Se) sites of NiSe. The imported Eu atoms could induce essential Ni 3d and Se 4p orbital reconstruction through gradient d-p-f coupling, thereby optimizing the band center alignment between NiSe and LiPSs. Such electronic reconstruction strengthens both d-p hybridization between Ni and LiPSs and s-p hybridization between Se and LiPSs, which can not only enhance the chemisorption affinity toward LiPSs but also accelerate interfacial charge transfer kinetics, leading to suppressed shuttle effect and boosted LiPSs conversion kinetics. Therefore, the Li-S batteries assembled with Eu incorporated NiSe deliver exceptional electrochemical performance with a high specific capacity of 896.2 mAh g-1 at 4 C and a retained areal capacity of 5.66 mAh cm-2 under a high sulfur loading of 5.94 mg cm-2 after 100 cycles. This work underscores the critical role of rare-earth 4f orbital coupling for modulating the active sites to construct high-efficiency electrocatalysts for Li-S batteries and beyond. (c) 2025 Science Press and Dalian Institute of Chemical Physics, Chinese Academy of Sciences. Published by Elsevier B.V. and Science Press. All rights are reserved, including those for text and data mining, AI training, and similar technologies.

Electrodeposited nickel is widely used in high-precision manufacturing, where both crystallographic orientation and internal stress critically affect the mechanical performance and dimensional stability of coatings. However, achieving simultaneous control over crystallographic orientation and internal stress remains a significant challenge in electroforming processes. In this study, a dual-additive strategy is proposed by combining PEG of various molecular weights (200, 2000, and 20,000) with sodium naphthalene-1,3,6-trisulfonate (NTS) to regulate both crystal orientation and internal stress in nickel coatings. Experimental results show that high-molecular-weight PEG-20,000 promotes (111) and (220) preferred orientations while suppressing the (200) plane, thereby improving coating hardness. Molecular dynamics simulations confirm that the polymerization degree of PEG correlates positively with its adsorption energy on Ni (111), which hinders vertical grain growth and promotes lateral expansion. However, PEG also significantly increases tensile stress by inhibiting the migration of nickel atoms and expanding interplanar spacing, as evidenced by both simulation and stress measurement. The introduction of NTS effectively compensates for this effect, reducing tensile stress and enabling the attainment of zero internal stress within the concentration range of 0-1 g/L. Furthermore, COMSOL simulations were conducted to optimize the circumferential current density distribution during the electroforming of Wolter-I type Xray focusing mirrors. The results show that uniform anode configuration improves current uniformity, reduces stress fluctuations, and helps prevent mirror deformation. This work provides an effective approach for the simultaneous regulation of texture and stress in nickel electroplating and offers practical guidance for fabricating high-performance, low-stress nickel coatings in high-precision manufacturing, such as X-ray optics.

Lithium iron phosphate batteries are widely adopted because of their cost-effectiveness. However, the large-scale recycling of these batteries is constrained by the economic and safety challenges posed by existing recycling technologies. Here, a sustainable and universal strategy based on low-temperature aqueous relithiation is proposed for LFP regeneration utilizing hydroxylamine sulfate as a mediator. The enhanced reductive environment created by hydroxylamine sulfate significantly lowers the Li+ migration energy barrier to lithium vacancies and enhances the repair of FeLi antisite defects at a reduced temperature of 40 degrees C, simplifying the operational process substantially. By combination with a short annealing step, the Li loss and structural degradation in LFP are effectively mitigated, enabling further restoration of electrochemical performance. Notably, the results of in situ X-ray diffraction (XRD) during the lithiation process reveal that the final step of complete lattice repair is a critical factor in controlling the lithium replenishment process. Furthermore, this process exhibits integration, sustainability, and universality, thereby overcoming the barriers to transitioning direct recycling from lab-scale to industrial applications.

Owing to their low cost and abundant resources, lignite-based hard carbons have been regarded as important candidates for practical sodium-ion batteries. To pursue high-rate properties in different electrolyte systems, their important microstructures are always designed. However, the effects of structural traits and electrolytes remain unclear on rate capability at different voltage regions, leading to inferior optimization in specific electrolyte systems. Herein, a series of lignite-based carbons are successfully prepared, displaying the significant evolution of tunable interlayer spacing, and closed-pores architecture. In ester-based electrolytes, the physical evolution plays an important role in Na+ diffusion behavior, especially the expanded interlayer spacing (∼4.00 Å). As a result, the HM-1000 electrode delivers 116.9 mAh g⁻1 at 4.0 C with a low decay of only 0.021% per cycle over 1000 loops. In contrast, for diglyme-based electrolytes, benefiting from intrinsic desolvation behavior, the physicochemical evolution could play a significant role, especially the formation of conductive films. The optimized HM-1400 delivers 345.9 mAh g−1 with 94.2% capacity retention after 1000 cycles and maintains 241.6 mAh g−1 at 4.0 C. Importantly, supported by ex situ Raman spectroscopy, DFT calculations, MD simulations and Pearson correlation analysis, the ion-transport behaviors in the sloping regions are determined by SEI properties, whilst those in the plateau region are governed by interlayer spacing and pore-filling nucleation energy. Therefore, this work establishes a microstructure-electrolyte matching guideline for lignite-derived hard carbon anodes in representative EC/EMC/DMC/diglyme electrolyte systems, providing a useful framework for the rational design of high-rate hard carbon anodes.

Aqueous zinc-iodine batteries (ZIBs) based on four-electron I-/I0/I+ redox chemistry hold great promise for high-energy-density energy storage. However, their practical deployment faces critical challenges, mainly including the polyiodide shuttle effect, hydrolysis of I+, sluggish iodine conversion kinetics and poor reversibility of Zn anodes. Herein, we propose a low-concentration electrolyte strategy by employing choline chloride (ChCl) as a dual-functional additive to achieve highly efficient four-electron ZIBs. It is demonstrated that Ch+ not only suppresses polyiodide shuttle by strong complexation but also stabilizes the ICl intermediate and regulates the I-Cl bonding strength to facilitate the subsequent conversion to I2 at the iodine cathode, thereby overcoming the key kinetic bottleneck of the I0/I+ redox process. Simultaneously, Ch+ facilitates Zn2+ transfer kinetics and inhibits water activity, effectively promoting uniform Zn plating with suppressed side reactions. Benefitting from these advantages, the ZIBs assembled with dilute ChCl deliver a high specific capacity of 445 mA h g-1 at 1 A g-1 and achieve 75% capacity retention after 50 000 cycles at a high current density of 10 A g-1. This work provides a facile strategy to simultaneously address the thermodynamic and kinetic issues to enable high-performance four-electron ZIBs.

The anisotropic electrical conductivity of unidirectional carbon fiber reinforced polymer (UD CFRP) laminates is important for electrically functional composite structures. This paper presents a multiscale modeling framework incorporating interlaminar conductive bridges to investigate laminate electrical behavior. At the micro-scale, a 3D resistor network model accounting for random fiber distribution and inter-fiber contact is established to predict the effective conductivity tensor. Subsequently, a meso-scale discrete fiber-bridging model is developed to characterize the interlaminar conductive pathways. Finally, the macroscopic electrical response is simulated using a homogenization strategy and validated through experimental characterization. The good agreement between numerical predictions and experimental measurements (with relative errors of 10.64% and 4.03% in the longitudinal and transverse directions, respectively) confirms the feasibility of the proposed model. The results reveal that the in-plane conductivity is primarily governed by the intrinsic properties of the fiber layers. The through-thickness conductivity exhibits a size effect associated with the specimen surface area (400-1600 mm2) and aspect ratio (0.25-4), arising from differences in the density of interlaminar conductive bridges. This work provides an efficient framework for interpreting the anisotropic electrical behavior of UD CFRP laminates and offers a useful basis for future extensions toward multifunctional composite design.

Light-mediated electronic spin modulation possesses intriguing potentials for photochemistry, enabling on-demand customization of catalysts towards distinct reactions and catalytic requirements. However, the significant photobleaching of the transient spin transitions as well as their temporal mismatch with slower chemical reaction dynamics substantially hinders its applicability. Herein, we demonstrate light-driven steady-state and on-demand catalyst spin modulation that effectively activates plasmonic catalysis. The rapidly oscillating plasmonic electromagnetic near-field spin-polarizes a low-spin CoFe2O4 catalyst and overcomes the photobleaching to produce stable high-spin states with astounding spin lifetimes >60 μs. The high-spin plasmonic catalyst effectively balances the tradeoff between spin polarization and carrier dynamics. For benchmark light-driven nitrate reduction catalysis, it achieves substantial photo-enhancement in ammonia production rate and selectivity as well as photocatalytic performance driven by sunlight, benefiting from polarization activation of nitrate reactant and preferential reaction pathway modulation. The highly generalized light-mediated strategy opens intriguing new avenues for on-demand and steady-state electronic spin engineering with profound implications for distinct disciplines.

Constructing in-plane cationic ordering in layered oxide cathodes can mitigate the adverse effects associated with the anionic redox reaction to achieve high energy density, while recent studies reveal that cationic disordering may also stabilize oxygen redox by tuning the local coordination environment of lattice oxygen. These findings underscore the pivotal role of local coordination and raise a further question regarding how the structural evolution of the transition metal sequence during electrochemical cycling dynamically dictates the charge compensation pathway. Herein, we unraveled the charge compensation evolution of P2-type Na0.6Li0.2Mn0.8O2 (NLMO) upon cationic ordering-disordering transition. During the initial cycle process, the electron holes are delocalized over oxygen ions coordinated to two Mn (O-Mn2) units arranged in the ribbon superstructure within the TM layers of NLMO, enabling a reversible anionic redox reaction. Upon extended cycles, the irreversible chemical depletion of Li and O serves as the thermodynamic driving force that destabilizes the ribbon superstructure. This structural instability facilitates in-plane Mn migration as a kinetic pathway, converting O-Mn2 units to O-Mn3 configurations and driving the macroscopic ordering-to-disordering transition. This fundamental structural disordering uniquely activates the bulk Mn2+/Mn3+ redox couple, which compensates for the diminished anionic redox contribution. By revealing the dynamic coupling between superstructure evolution and redox behavior, this work identifies irreversible cationic transitions as the root cause of structural degradation, underscoring the necessity of constructing rigid TM frameworks in high-capacity layered cathodes.

Constructing electrocatalysts with heterostructures has emerged as an efficient approach to cooperatively catalyze the conversion of lithium polysulfides (LiPSs) in lithium-sulfur (Li-S) batteries. However, it remains a formidable challenge to fundamentally understand the structure-activity relationship between the interfacial configuration and electrocatalytic performance, which is crucial for the rational design of electrocatalysts with heterojunctions. Herein, by leveraging molybdenum carbides (MoxC) with tunable crystal structures as model electrocatalysts, we systematically investigated the geometric-configuration-dependent catalytic activity for LiPS conversion. Experimental analyses confirmed that the cubic MoC with octahedrally coordinated Mo atoms (Mooct) is easily passivated because of its robust LiPS affinity, while the hexagonal Mo2C with triangularly coordinated Mo atoms (Motri) functions better in improving the interfacial charge transfer. Accordingly, the constructed heterointerfaces integrated with dual-geometric coordination endow MoC/Mo2C with moderate LiPS adsorption and favorable charge transfer kinetics to cooperatively catalyze LiPS conversion. Benefiting from these advantages, the Li-S batteries assembled with MoC/Mo2C demonstrate superior reversible specific capacities and cycling durability. This work highlights the critical role of interfacial geometric coordination in heterojunctions for LiPS retention and catalysis, offering a guiding approach for elevating the activity of heterojunction electrocatalysts.

ABSTRACT Hard carbon (HC) is a promising anode candidate for sodium‐ion batteries (SIBs), yet its application is plagued by unstable interfaces and poor long‐term cyclability. Herein, we develop a facile solvent evaporation strategy to synthesize ultrathin Al 2 O 3 ‐coated biomass‐derived HC (GSC‐Al 2 O 3 ‐3%). The conformal Al 2 O 3 layer passivates defects and micropores, suppresses side reactions, and promotes the formation of a robust organic–inorganic hybrid solid electrolyte interphase. Comprehensive characterizations, including in situ X‐ray diffraction, ex situ Raman spectra, X‐ray photoelectron spectroscopy, time of flight secondary ion mass spectrometry, solid‐state 27 Al nuclear magnetic resonance, and atomic force microscope modulus mapping, demonstrate that Al 2 O 3 actively participates in SEI reconstruction, enhancing the chemical and mechanical stability. Electrochemical tests reveal that the optimized GSC‐Al 2 O 3 ‐3% anode delivers 91% capacity retention after 1000 cycles at 1.0 A g −1 , and possesses excellent wide‐temperature tolerance (149.3 mAh g⁻¹ at −30°C and 286.8 mAh g −1 at 60°C). Mechanistic studies confirm a synergistic Na + storage process involving “adsorption–intercalation–pore filling,” while density functional theory calculations and electrostatic potential mapping reveal that Al 2 O 3 coating regulates interfacial charge distribution and reduces Na + migration barriers. A full cell paired with a NaNi 0.5 Fe 0.5 MnO 4 cathode exhibits a high initial capacity of 395.7 mAh g −1 and outstanding cycling stability (200 cycles). This work provides fundamental mechanistic insights into interfacial engineering of HC and establishes a cost‐effective, scalable route for the next generation high‐performance SIBs.

DNA hydrogels are promising platforms for portable biosensing, but their combination with high-activity catalytic nanomaterials remains hindered by interfacial incompatibility and inconsistent device-level retention. Here, a tube-anchored hydrogel microreactor is developed, coupling Co-Ni dual-atom nanozymes (CoNi DANs), interfacial stabilization, and CRISPR-triggered release within a standard centrifuge tube. CoNi DANs are synthesized on a defect-rich nitrogen-doped carbon scaffold, achieving high metal loading and improved peroxidase-like activity relative to those of their single-atom counterparts. Carboxymethyl cellulose-mediated interfacial stabilization then suppresses CoNi DAN aggregation through electrostatic complementarity and polymeric steric shielding, enabling uniform dispersion of CoNi DANs within the DNA hydrogel. A polydopamine-based dual-anchoring strategy further combines covalent grafting with sequence-specific DNA hybridization, providing a chemically reinforced hydrogel-device interface. Upon target recognition, CRISPR/Cas12a trans-cleavage activity induces controlled hydrogel degradation and on-demand release of CoNi DANs for colorimetric and electrochemical dual-mode readout. Using atrazine as a proof-of-concept analyte, the platform achieves limits of detection of 6.1 and 2.1 pg mL-1 for colorimetric and electrochemical modes, respectively, with satisfactory recoveries in real samples. A smartphone-assisted digital readout module further improves the portability of the colorimetric mode. The dual-interface design, uniting material-level compatibilization with device-level dual-anchoring, provides a generalizable framework for embedding high-activity nanozymes into responsive DNA hydrogel microreactors for portable on-site biosensing.