Nanoconfined water exhibits unique properties compared to bulk water due to limited quantities, frustrated hydrogen bonding, and surface interactions, which are fundamental for energy storage and transport applications. We integrate machine learning-accelerated ab initio molecular dynamics with x-ray diffraction (XRD) and inelastic neutron scattering (INS) to systematically analyze the thermodynamic and dynamic behavior of water confined between functionalized (-F, -O, and -OH) two-dimensional (2D) Ti3C2Tx MXene layers. As water intercalates between layers, the interlayer spacing exhibits layer-dependent staging characteristics. The water polarization can be flipped by the count and morphology of intercalated molecules interacting with MXene surface groups, resulting in varying electrostatic potential profiles. On the basis of interfacial electrostatic potential, hydrogen bond lifetime, and molecular orientation, we establish a linear combination of exponential model describing water diffusivity. These computational insights align well with experimental x-ray and neutron measurements, suggesting strategies for tuning water morphology and transport by tailoring MXene surface chemistry and water content for electrochemical energy storage and nanofluidic applications.

Magnesium-based materials are promising for solid-state hydrogen storage, yet their practical application is impeded by the high thermodynamic stability of MgH₂ and sluggish sorption kinetics. Here, we develop a targeted interfacial engineering strategy via d-band modulation to tailor the hydrogen storage performance of nano-Mg, by fabricating hexagonal boron nitride-supported PdNi bimetallic clusters (PdNi/BN) as an advanced catalytic additive. The nano-Mg@PdNi/BN composite delivers a drastically reduced onset dehydrogenation temperature of 173 °C (175 °C lower than pristine MgH₂), along with ∼95% capacity retention over 10 cycles. Kinetic and thermodynamic analyses confirm the composite exhibits remarkably lowered hydrogen absorption/desorption activation energies and reduced hydride formation enthalpy. Density functional theory calculations reveal that strong interfacial interactions at the PdNi/BN interface downshift the PdNi d-band center to −1.456 eV, which weakens Mg-H bonds, lowers hydrogen vacancy formation energy to −0.598 eV, and enhances H₂ absorption, enabling a bifunctional catalytic effect for both hydrogen sorption processes. This work provides a powerful strategy and atomic-level guidance for designing high-performance Mg-based hydrogen storage materials via d-band modulation.

Graph neural networks (GNNs) inherently excel at representing atomistic material, therefore enabling predictions of properties with high accuracy with embedded descriptors. Approaching to accurate prediction of a variety of physical properties of diverse materials, particularly those with multicomponents, remains challenging due to the complexity of many-body atomic interactions and the reliance on handcrafted symmetry descriptors. Here, we introduce the Wavelet Atomic Neighborhood Network (WANN), a novel framework that implicitly captures many-body interactions through an iterative subembedding module for updating atomic features, thereby eliminating the integration of the predefined feature engineering. A wavelet-based regression component is built up through multiscale feature analysis. WANN demonstrates superior accuracy, achieving small mean absolute error (MAE) in predicting a variety of physical and chemical quantities, including thermodynamical, dielectric, piezoelectric, magnetic, and thermoelectric properties. For instance, it could significantly reduce MAE maximum by 61.64% in comparison to Matformer for shear moduli and by 90.84% in comparison to ALIGNN for the exfoliation energy. This scalable and preprocessing-light deep-learning framework provides an efficient toolkit for facilitating high-throughput screening of emergent materials, like high-entropy alloys and ceramics.

Solid-state electrolyte lithium (Li) metal batteries have been considered as promising storage devices due to their high energy density, good thermal stability and safety. The key to achieving their superior performance lies in maintaining a stable solid-solid interface. Although applying high pressure is a common strategy to improve interfacial contacts, the generally poor pressure tolerance of the Li metal anode has largely been overlooked by researchers. Under high pressure, the Li anode undergoes significant volume changes and creep, which not only fails to maintain intimate contact but also intensifies interface separation, ultimately leading to performance degradation. Herein, a gel polymer electrolyte (GPE)/Li metal/carbon fiber cloth (CFC) composite anode (G-LiCFC) with high pressure resistance capability was fabricated by the hot-melting method. The G-LiCFC composite anode not only maintains structural integrity under a high pressure of 30 MPa but also contributes to forming an excellent interface with the electrolyte. As a result, the symmetric cells of the G-LiCFC composite anode display stable cycling for 4870 hours at a high areal capacity of 12 mA h cm-2, and the LiFePO4|GPE|LiCFC full cells exhibit excellent cycling performance with no capacity decay after 410 cycles at 0.2 C under a high pressure of 10 MPa.Keywords: Solid-state electrolyte; Li metal; Carbon fiber cloth/lithium metal composite; Compressive resistance; Interface.

Aqueous zinc-ion batteries (AZIBs) are gaining momentum as a promising secondary battery technology due to their high safety, environmental friendliness, abundant resources, and competitive energy density. These attributes position them as viable alternatives to traditional lithium-ion batteries. However, the commercialization of AZIBs faces significant challenges, including high desolvation barriers that complicate ion mobility, sluggish ion-transport kinetics, zinc dendrite growth, and detrimental side reactions. To address these issues, there has been a growing interest in utilizing biomass-based materials in the design of advanced AZIBs. These materials inherently possess excellent hydrophilicity, strong mechanical strength, and abundant active functional groups, all of which can enhance the performance of AZIBs. This review offers an in-depth examination of current progress, prevailing limitations, and potential solutions for biomass-derived electrode materials to achieve enhanced long-cycle stability and rapid electrochemical kinetics in AZIBs. Furthermore, this review systematically addresses pivotal issues and emerging research directions concerning the design of zinc anodes, while guiding the future optimization of AZIBs with exceptional electrochemical performance. Hence, it furnishes a comprehensive outlook on the prospective evolution of biomass-based AZIBs, while highlighting critical challenges, and opportunities that may accelerate their ongoing development, and facilitate their wider adoption in practical applications.

The recently emerging heterojunctions with remarkable thermal effects and chemical bonding have attracted intensive attention due to their fast photocarrier separation and transportation. Herein, quasi-zero-dimensional carbon quantum dot (0D CQD) with multi-functional groups is adopted to in situ construct a superhydrophilic heterojunction on electron-deficient Se-doped ZnCdS (Se-ZCS) via amide linkages. Sulfur vacancies in Se-ZCS serve as electron reservoirs, and photothermally active CQD function as hydrophilic components, light capturers, and electron acceptors, while the amide bond channels promote the smooth carrier transfer across the Se-ZCS/CQD interface. Simultaneously, the interfacial electronic barrier prohibits the photoelectron transfer to Se-ZCS. Thereby, the formed Se-ZCS/CQD heterojunction successfully elongates the photoelectron lifetime to drive efficient photothermal catalytic reactions. Particularly, optimal Se-ZCS/CQD achieves a 2-fold increase in H2 production (126.8 mmol gcat-1 h-1) compared to pure Se-ZCS under visible light irradiation, surpassing the majority of reported ZnCdSbased photocatalysts. More importantly, it exhibits exceptional long-term stability with only a decline of 8.07% after 16 h of testing. The expanded application of Se-ZCS/CQD in the pretreatment of wastewater presents a removal efficiency of similar to 96.5% after 2 h. The strategy provides anew idea for designing chemical contact between semiconductor and photothermal active materials, and for realizing efficient photocatalysis by improving charge separation and transfer. (c) 2026 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.

MXenes are emerging as highly promising supercapacitor electrodes. However, the synergistic effects of their diverse surface terminations and transition metals on intrinsic and electrochemical capacitances remain elusive. Establishing a theoretical pipeline will be beneficial to efficiently understand the capacitive behavior and design high-performance materials. Here, we employ first-principles calculations in combination with the rigid band approximation (RBA) and constant potential free energy (CPFE) methods to perform a systematic investigation of the capacitive behavior via synergistic regulation of surface terminations and transition metals in M3N2T x (M = Ti, V, Zr, Nb, Mo, Hf, Ta, W; T x = O, S, Se, F, Cl, Br). The O-, S-, and Cl-terminated ones exhibit higher quantum capacitance performance than the others. A metal group-descending and period-ascending trend in capacitance is concluded. Moreover, the electrochemical capacitance is primarily governed by the electronegativities of the surface groups and changes in bond lengths. The combination of intrinsic and electrochemical capacitances achieves an optimal trade-off between computational efficiency and accuracy. Several candidates are predicted to possess both high capacitance and energy density, e.g., V3N2O2 (167 F/g, 33.5 Wh/kg) and Ti3N2O2 (163 F/g, 32.7 Wh/kg). Overall, we establish a full-spectrum evaluation paradigm that bridges electronic structure, interfacial phenomena, and capacitive performance, overcoming the limitations of conventional single-method studies and offering a robust theoretical foundation and predictive toolkit for the rational design of next-generation energy storage materials.

ABSTRACT The growing demand for low‐temperature lithium metal batteries in aerospace, polar exploration, and other extreme environments calls for polymer electrolytes that can maintain efficient ion transport and interfacial stability under cryogenic conditions. Yet the low‐temperature application of polymer electrolytes is typically limited by the strong coupling of Li + transport to sluggish polymer segmental relaxation, leading to severe polarization, slow desolvation, and unstable electrode interphases. Here, we report an ion‐transport topology engineering strategy based on an in situ polymerized poly(1,3‐dioxolane) (PDOL) electrolyte. By introducing fluorobenzene (FB) as a hydrogen‐bond‐guided molecular organizer, we create a preorganized local transport field that weakens excessive Li + ‐ether oxygen coordination and reconfigures the local Li + migration landscape. This topology‐engineered microenvironment promotes anion‐rich coordination, lowers desolvation barriers, and directs inorganic‐rich interphase formation on both Li metal and high‐voltage cathodes. Consequently, the optimized electrolyte delivers a Li + transference number of 0.76 at −40°C and stable operation from −65 to 25°C. Li||Li cells cycle over 2000 h at −40°C, Li||LiNi 0.8 Co 0.1 Mn 0.1 O 2 coin cells retain 99% capacity after 320 cycles, and pouch cells retain 84.9% after 450 cycles. This work establishes ion‐transport topology engineering as a viable design principle for polymer electrolytes under extreme‐temperature conditions.

With the development of clean energy systems, more efforts have been put into aqueous zinc-ion batteries (AZIBs), originating from its high safety and low cost. However, cathode materials still face challenges such as low capacity, poor cycling stability, and a lack of active sites at high potentials. This study proposes a covalent organic framework material (TABQ-TFP-COF) containing dual active sites, which has been successfully applied for AZIBs. It exhibits excellent structural stability, low solubility, and rapid ion transport capabilities. With an electrolyte system containing Mn2+ additives, TABQ-TFP-COF cathode demonstrates a high specific capacity of 264 mAh g-1 (at 0.1 A g-1) and a capacity retention rate close to 100% in 1500 cycles (at 1 A g-1), along with outstanding rate performance. Through systematic characterization methods, including in situ FTIR, ex situ XRD, and XPS, combined with theoretical calculations, the reversible co-intercalation mechanism of H+/Zn2+ at C=O/C=N sites is revealed. Additionally, pouch cells assembled based on this material maintain stable voltage output under various mechanical deformation conditions. This study offers design strategies for high-performance AZIBs and provides mechanistic insights into multi-ion energy storage.

Potassium-ion batteries (KIBs) have emerged as promising, cost-effective alternatives to lithium-ion batteries. However, their practical viability is still hampered by persistent instabilities associated with cathode materials and their interactions with electrolytes. This review provides a mechanism-focused perspective on this challenge. We begin by summarizing the principal families of inorganic cathode materials with their corresponding electrolyte systems. Then, three coupled degradation mechanisms are highlighted: (i) lattice distortion and irreversible phase transitions arising from the large ionic radius of K+, (ii) oxygen release and transition-metal (TM) dissolution that accelerate electrolyte decomposition, and (iii) the dynamic formation, reconstruction, and failure of the cathode-electrolyte interphase (CEI). Recent progress in optimization strategies, including defect engineering (aliovalent doping and vacancy regulation), surface engineering, nano engineering, and electrolyte engineering, is critically evaluated with respect to their ability to suppress structural degradation, limit TM loss, and engineer robust CEIs. Finally, we discuss future directions, emphasizing the need for integrated approaches that combine theory and rational electrolyte design to achieve a durable CEI and crystal stability of the desired inorganic cathode material, in turn, leading to predictive control over long-term electrochemical behavior.

The practical deployment of lithium–sulfur (Li–S) batteries is hampered by the shuttle effect of lithium polysulfides (LiPSs) and sluggish kinetics of sulfur redox reaction. While prevailing research focuses on maximizing the intrinsic activity of catalysts, the critical role of the host architecture in modulating the local reaction microenvironment remains overlooked. Herein, we report a facile ion-exchange strategy to synthesize double-shell hollow Prussian blue analogue derivative (Co2.5Fe/NC) as advanced sulfur hosts by precisely controlling the Co/Fe molar ratio at 2.5. Finite element simulations and in situ diagnostics reveal that the double-shell structure orchestrates a self-propelled electrolyte flow within the nanoreactor during operation. This dynamic flow effectively mitigates the spatial concentration heterogeneity of LiPSs, especially near the catalysts, thereby preventing active material passivation and ensuring sustained high catalytic efficiency. Consequently, even with a catalyst of moderate intrinsic activity, the Co2.5Fe/NC cathode achieves exceptional stability under lean electrolyte conditions (0.016

The electron spin state of transition metal ions represents a fundamental quantum property that is increasingly recognized as a pivotal design dimension for tuning the performance of cathode materials in Li/Na/K‑ion batteries. This review begins by consolidating the foundational principles through which spin states govern electrochemical properties, establishing a robust theoretical framework that bridges atomic-scale coordination environments with macroscopic electrode behavior. It further discusses advanced experimental and computational techniques for probing complex spin states and, critically, for establishing clear structure-spin-performance relationships. A central focus is placed on the rational design of spin configurations, whether via proactive engineering or suppression of unfavorable transitions, to optimize key electrochemical processes: modulating cationic vs. anionic redox competition, enhancing structural stability by mitigating Jahn-Teller distortions and magnetic frustration, and improving charge and ion transport. The review also highlights the emerging role of spin‑sensitive machine learning as an accelerated pathway for discovering superior cathode materials. By integrating theoretical insights, methodological advances, and application‑oriented studies, this work provides a comprehensive mechanistic framework and practical guidelines for the design of next‑generation high‑performance cathodes through deliberate spin‑state control.

Germanium (Ge) is a promising high-capacity anode material for lithium-ion batteries; however, its practical application remains limited by substantial volume variation, unstable interfacial reactions, and rapid capacity degradation during repeated lithiation/delithiation. In this work, a binder-free Ge/C/MXene@NF hybrid electrode was developed through a sequential fabrication process, where Ge nanoparticles were immobilized within a PVP-derived carbon matrix supported on a three-dimensional nickel-foam scaffold and subsequently integrated with a Ti3C2Tx MXene conductive network to construct a hierarchical Ge/C/MXene hybrid architecture. The nickel foam provides a continuous current-collecting framework and mechanical support, while the MXene network improves electrical connectivity, electrolyte accessibility, and interfacial charge-transfer kinetics. Structural and compositional analyses further indicate the presence of PVP-derived carbon and a possible minor NiGe interfacial phase formed during annealing. Comparison with Ge@NF and the individual component electrodes provides insight into the respective contributions of MXene, Ge, and the PVP-derived carbon framework to the electrochemical behaviour of the composite electrode. Using the total deposited active-material mass as the normalisation basis, the MXene@Ge@NF electrode retains a reversible specific capacity of 789.8 mAh g−1 after 100 cycles at an effective current density of 76.2 mA g−1. The observed electrochemical behaviour originates from the integrated contributions of Ge nanoparticles, the PVP-derived carbon matrix, the conductive Ti3C2Tx MXene network, the three-dimensional nickel-foam scaffold, and possible Ni–Ge interfacial interactions. Rather than representing a Ge-dominated electrode, this architecture demonstrates the advantages of integrating multiple functional components within a binder-free Ge/C/MXene hybrid architecture.

Lithium-metal batteries (LMBs) are considered among the most promising high-performance energy storage systems because lithium metal possesses extremely high theoretical capacity and the lowest electrochemical potential among anode materials. However, their practical implementation remains severely limited by several critical challenges at the nanoscale, including uncontrolled lithium dendrite growth, unstable solid-electrolyte interphase formation, low Coulombic Efficiency, and large volume fluctuations during repeated lithium plating and stripping processes. In recent years, nanostructured porous framework materials have emerged as effective host structures and interfacial regulators for stabilizing lithium metal anodes due to their high surface areas, tunable pore architectures, and functionalizable chemical environments. In this review, we systematically summarize the recent progress in metal–organic frameworks (MOFs), covalent organic frameworks (COFs), covalent organic polymers (COPs) and other organic framework materials for lithium-metal anode applications. First, the fundamental working principles of LMBs and the major challenges associated with lithium metal anodes are discussed. Subsequently, the structural characteristics and advantages of MOFs, COFs, COPs and other framework materials are compared, followed by a detailed discussion of lithium storage mechanisms in porous frameworks, including lithium adsorption and nucleation, regulation of plating and stripping, dendrite suppression, and stabilization of the solid electrolyte interphase. Key design strategies, including hierarchical pore engineering, lithiophilic chemical functionalization, and electronic conductivity enhancement, are systematically highlighted. Representative advances in COF-based, MOF-based, and COP-based materials for lithium metal stabilization are critically summarized and compared. Finally, the remaining challenges and future research directions for porous framework materials in LMBs are discussed. This review aims to provide fundamental insights and design strategies for the rational development of advanced porous framework materials toward safe, stable, and high-energy LMBs.

As porous crystalline materials, covalent organic frameworks, containing an abundant porous structure, can be adopted as host materials for gas adsorption. A series of functionalized covalent organic framework materials, including methoxy-modified COF-A-OMe and vinyl-modified COF-A-Vinyl, have been constructed to compare with original COF-A in terms of regulation of topology and thermal stability. Upon application for CO2 adsorption, improved adsorption properties have been achieved for COF-A-OMe and COF-A-Vinyl materials with functional group modification. This can be ascribed to the large specific surface area and enhanced pore volume of modified COF materials as well as the optimized adsorption advantages based on the interaction between modified functional groups and CO2 molecules. Although a physically dominated adsorption mechanism existed for COF-A, COF-A-OMe, and COF-A-Vinyl, the synergistic role of -C═N- and -CH═CH2 groups in COF-A-Vinyl for CO2 adsorption has been confirmed based on density functional theory (DFT) simulation. This work can extend the application of organic frameworks for gas adsorption with a rational structure design or functional modification.

Lithium metal anodes (LMAs) are regarded as the "holy grail" for next-gen high-energy batteries, yet their practical use is hampered by dendrite growth, infinite volume expansion, and interfacial instability. Three-dimensional...

Wet-spinning is an effective and scalable continuous manufacturing process for fiber electrodes. However, fiber electrodes prepared by traditional wet-spinning often suffer from low mechanical strength and poor ionic/electronic conductivity. Inspired by the radially hierarchical structure of plant stems, we developed a coaxial wet-spinning technique based on a drawing-extrusion mechanism. By regulating the Ca2+ concentration in the coagulation bath, a core-pith-sheath tri-layer architecture was constructed, which synergistically enhances mechanical strength and establishes efficient ionic transport pathways. Besides, a composite cathode consisting of MnO2 nanosheets anchored on carbon nanotubes (CNTs) was synthesized, establishing a continuous electronic conducting network. The incorporation of dual conductive networks markedly enhanced the electrochemical and mechanical properties of the fiber electrodes. The fabricated fiber-shaped Zn-MnO2 batteries (FZBs) delivered capacities of 343.5 mAh & centerdot;g-1 at 0.1 A & centerdot;g-1 and 144.7 mAh & centerdot;g-1 at 5 A & centerdot;g-1, respectively, along with excellent cycling stability-retaining 55.2% capacity after 5000 cycles at 5 A & centerdot;g-1 (an average per-cycle decay of 0.01%). Moreover, after 100,000 bending cycles at 2 A & centerdot;g-1, the capacity retention remained 74.9%. Furthermore, through tomography, electrochemical kinetics analysis, and ion-transport theoretical simulations, we elucidated the critical role of rapid ion migration within the porous pith layer in enabling high performance fiber batteries. The universality of this mechanism was further verified in aqueous fiber-shaped lithium-ion batteries. This work provides a scalable multilayer structural design strategy and theoretical foundation for the development of advanced fiber-based energy storage devices.

Electrocatalytic water splitting offers a sustainable route for converting renewable electricity into green hydrogen. Transition-metal-based layered double hydroxide (LDH) catalysts are considered attractive candidates for oxygen evolution reaction (OER) catalysis. Nevertheless, their catalytic performance remains constrained by poor conductivity, limited affinity for oxygen intermediates, and unsatisfactory durability. Here, we report a self-supported Ce-doped Co alloy/NiFe layered double hydroxide heterostructure on carbon fiber paper (CoCe/NiFe-LDH/CP) fabricated by two-step electrodeposition, which owns a hierarchical fiber-nanoflower-nanoparticle architecture, and provides a hydrophilic/aerophobic surface. The optimized electrode delivers overpotentials of 190 and 249mV at 10 and 100mAcm-2 with stable operation for 120h and a Tafel slope of 27.4mV dec-1. The characterization results show that the establishment of the alloy/NiFe-LDH heterostructure enhances electrical conductivity while Ce doping strengthens the electronic coupling at the heterointerface and induces lattice distortion in the Co phase, thereby optimizing the adsorption behavior of oxygenated intermediates during OER, achieving synergistic regulation of electrical conductivity and oxygen-intermediate adsorption. Density functional theory further shows a reduced barrier for the Gibbs free energy together with a more appropriate interfacial d-band center, suggesting optimized intermediate binding at the alloy/LDH interface. This rare-earth-enabled alloy/LDH interface strategy provides a reference for designing high-performance OER anodes through coupled alloying and heterointerface engineering, offering a more integrated route than conventional single-factor optimization in OER catalysts.

The buried interface between perovskite and SnO2 is plagued by defects and voids, limiting n-i-p solar cell performance. It is challenged for interfacial modification such as potassium salts to simultaneously passivate defects and modulate the buried PbI2·DMSO adduct. Here, we introduce a heterocyclic potassium salt, acesulfame potassium (Ace-K), with dual C═O and -SO2- groups for defect passivation and competitive ligand modulation. Ace-K anchors uncoordinated Sn4 + and oxygen vacancies on SnO2 via bidentate chelation. During PbI2 deposition, Ace-K competes with DMSO for PbI2, reducing PbI2·DMSO at the SnO2/perovskite interface. This reduction leads to a void-free perovskite bottom interface. Concurrently, it promotes DMSO escape to create a porous PbI2 structure, which facilitates organic salt penetration and yields high-quality perovskite films with released residual stress. Ace-K remaining at the interface enhances charge transfer kinetics. Consequently, the champion device (0.0729 cm2) achieves a lab-measured PCE of 26.17% with an open-circuit voltage of 1.19 V. The heterocyclic structure also imparts UV resistance, and the devices retain 92.4% of their initial efficiency after 1000 h of maximum power point tracking under continuous illumination. This work demonstrates a competitive ligand modulation strategy, offering a microstructural pathway toward efficient and stable perovskite photovoltaics.