Amid the global drive toward clean and cost-effective energy development, lithium-ion batteries (LIBs) have emerged as a cornerstone technology due to their high energy density and long cycle life, underpinning applications ranging from electric vehicles to portable electronic devices. However, the detrimental effect of low temperatures on lithium-ion battery performance remains a critical challenge, which demands urgent solutions at present. In this work, we designed a low-temperature fluorinated electrolyte, denoted LTDFM, by incorporating methyl difluoroacetate (MDFA), a fluorinated cosolvent with an ultralow melting point, into a dimethyl carbonate (DMC)/fluoroethylene carbonate (FEC) (8:2 v/v) base. This formulation was further enhanced with a dual-salt system of LiPF6 and bis(trifluoromethanesulfonyl)imide (LiTFSI) at a 6:4 molar ratio (1.0 M total salt concentration). The resulting LTDFM electrolyte enables not only stable long-term cycling performance at room temperature but also excellent electrochemical performance at a low temperature of -30 degrees C. This low temperature tolerance is attributed to the formation of a denser and mechanically robust solid electrolyte interphase (SEI) film rich in LiF, which effectively suppresses the growth of lithium dendrites and parasitic side reactions. This work provides valuable mechanistic insights and a practical strategy for designing high-performance low-temperature electrolyte for LIBs in extreme environments.

Despite their promising potential, the advancement of zinc-ion hybrid supercapacitors (ZHSCs) is significantly impeded by sluggish zinc-ion migration, parasitic side reactions, and dendrite growth, challenges that are exacerbated under low-temperature conditions. Current research predominantly focuses on zinc ions, while the critical role of anions in mediating these degradation pathways has been largely overlooked. Herein, we present a "cation group-driven dual-track regulation" strategy by engineering a cationic hydrogel electrolyte composed of poly(acryloyloxyethyl trimethyl ammonium chloride) (PDAC) and ZnCl2. The immobilized quaternary ammonium groups (─N+(CH3)3) electrostatically confine Cl‒ anions, thereby creating highly efficient Zn2+-selective migration channels and suppressing competing side reactions. Simultaneously, these cationic groups adsorb onto high-energy zinc crystal facets, guiding (002)-oriented Zn deposition and effectively inhibiting dendrite growth. The optimized PDAC-based electrolyte delivers a high ionic conductivity of 5.3 mS cm-1 at -50°C, a Zn2+ transference number of 0.87, and exceptional average reversibility of Zn plating/stripping (98%) in Zn||Cu cells down to -40°C. Moreover, PDAC-optimized ZHSCs demonstrate outstanding cyclability over 20 000 at -40°C (95.2% capacity retention). This work establishes a generalizable electrolyte design paradigm that concurrently addresses kinetic and interfacial limitations, paving the way for dendrite-free, high-performance Zn-based energy storage systems operable under low-temperature conditions.

Solving the problems of carbon dioxide(CO2)emis-sions and energy scarcity by the development of highly selective,cost-effective,and reliable catalysts for the electrochemical reduc-tion of CO2 to useful carbon-based products would be very helpful.We report the synthesis of an efficient graphene-supported bismuth single-atom catalyst(BiSA-G)featuring a BiN4 coordination struc-ture for this purpose.The synthesis used tannic acid as a multifunc-tional ligand and ammonia as a nitrogen dopant.Using a scalable coordination chemistry approach,BiN4 sites were uniformly dis-persed on the graphene substrate and were found to have an out-standing ability for the conversion of CO2 to CO,with a high Fara-daic efficiency of 97.4%at-0.55 V(vs.RHE)and a high turnover frequency of 5230 h-1 along with outstanding stability.Density functional theory calculations confirmed that the BiN4 site serves as the dominant active center,simultaneously facilit-ating CO2 activation and the efficient formation of the crucial intermediate*COOH with a reduced free energy barrier.This dis-covery offers a new way for the atomic-scale design of high-efficiency catalysts for the electrochemical CO2 reduction reaction,potentially helping sustainable carbon use.

Hematite (α-Fe2O3) is a promising photoelectrocatalyst for water oxidation, yet it suffers from intrinsic limitations including poor electrical conductivity, low charge-separation efficiency, an ultrashort hole-diffusion length, and a high onset potential, which hinder its practical performance. While constructing the Fe2O3/Fe3O4 heterojunction has proven effective in enhancing the photoelectrochemical properties of hematite, severe charge recombination at the heterojunction/electrolyte interface remains a critical challenge. In this work, a controllable synthesis strategy was employed to fabricate a series of core-shell Fe2O3/Fe3O4 heterojunction (T-ASSt@Cx) photoanodes with precisely tuned carbon-layer thicknesses using anodized stainless steel (T-ASSt) as the substrate. Through systematic investigations, a dual-regulatory function of the carbon overlayer on the photoelectrochemical performance was revealed. Specifically, an optimal moderate carbon layer (2-3 nm) could simultaneously passivate surface defects and serve as an efficient electron-extraction and transport pathway, significantly enhancing the charge-separation efficiency of the heterojunction from 47.7% to 83.7% at 1.23 V vs RHE and inducing a 360 mV cathodic shift in onset potential. In contrast, insufficient carbon layer thickness fails to suppress surface charge recombination, while excessive thickness severely hinders electrolyte access to the heterojunction and impedes hole transfer kinetics. DFT calculations demonstrate that the carbon nanolayer optimizes the adsorption of OER intermediates, significantly reduces the reaction energy barrier, and promotes charge transfer kinetics through interfacial electron redistribution. This study not only elucidates the critical balance between charge separation and mass transport governed by carbon overlayer thickness, but also provides interfacial engineering strategies for the rational design of high-performance, stable carbon-encapsulated heterojunction photoelectrocatalytic systems.

Prelithiation plays a critical role in compensating initial lithium loss in lithium-ion batteries (LIBs), yet achieving precise and uniform lithium compensation remains a significant challenging. Mechanical prelithiation faces challenges in fabricating ultrathin lithium foils, while lithium metal powder suffers from agglomeration and safety issues due to its high surface area. Chemical methods often form overly thick SEI films that hinder ion transport, and cathode additives like Li2O2 can release oxygen, causing gas evolution and accelerated capacity fade. These challenges highlight the need for more controlled and safer prelithiation strategies. Herein, we propose a short-circuit prelithiation method via electroplating to fabricate a composite anode featuring a tunable lithium layer (15-20 mu m) on copper foil. By optimizing the plating current, we precisely regulate the lithium thickness and facilitate spontaneous lithiation during subsequent aging period, leading to the formation of a stable inorganic-rich SEI. The optimized anode (preGr-30) exhibits a high initial Coulombic efficiency of 90.13% and outstanding capacity retention of 156.8% over 500 cycles. Mechanistic studies reveal that the pre-formed SEI dominated by LiF and Li2CO3 enhances interfacial ion transport and suppresses electrolyte decomposition. This work provides an efficient and scalable prelithiation strategy for advancing high-energy-density LIBs.

Iron-based Prussian blue (Fe-PB) materials have been widely investigated as cathode materials for sodium-ion batteries owing to their unique open framework structure. However, the enhancement of electrical conductivity and the reduction of structural defects in Prussian blue analogues remain challenging. In this study, hollow layered Fe-PB materials with gradually inward-etched centers were successfully synthesized through a phthalic acid (PA)-assisted chelation and etching process. Compared to conventionally hydrothermally synthesized materials, the prepared Fe-PB was characterized by an increased specific surface area, shortened sodium-ion diffusion pathways, and reduced lattice water content, leading to significantly improved electrochemical properties. When evaluated as a cathode material for sodium-ion batteries, the etched Fe-PB demonstrated an initial specific capacity of 106.4 mAh g- 1 at a current density of 100 mA g- 1. After 500 charge/discharge cycles, a specific capacity of 78.8 mAh g- 1 was maintained, corresponding to a capacity retention rate of 74.1 % and a remarkably low capacity decay rate of 0.05 % per cycle. This work not only provides an effective strategy for improving the sodium storage performance of Fe-PB materials but also offers valuable insights into the hydrothermal synthesis of high-performance Prussian blue analogues with reduced lattice water content and enhanced electrochemical properties.

The utilization of nickel-based catalysts as alternatives to expensive platinum-based(Pt-based)materials for the hydrogen evolution reaction in acidic electrolytes has attracted considerable attention due to their potential for enabling cost-effective industrial applications.However,the unsatisfied cyclic stability and electrochemical activity limit their further application.In this work,nickel-molybdenum(Ni-Mo)alloy catalysts were successfully synthesized through a comprehensive process including electrodeposition,thermal annealing,and electrochemical activation.Owing to the synergistic interaction of molybdenum trinickelide(Ni3Mo)and molybdenum dioxide(MoO2)in Ni-Mo alloy,the catalyst display superior overall electrochemical properties.A low overpotential of 86 mV at 10 mA/cm2 and a Tafel slope of 74.0 mV/dec in 0.5 mol/L H2SO4 solution can be achieved.Notably,remarkable stability with negligible performance degradation even after 100 h could be maintained.This work presents a novel and effective strategy for the design and fabrication of high-performance,non-precious metal electrocatalysts for acidic water electrolysis.

Electrocatalytic conversion of carbon dioxide (CO2) to formate is an effective strategy for converting CO2 into valuable chemicals. However, synthesizing active catalysts with well-defined heterojunctions and large exposed surfaces remains challenging. Here, we present a one-pot synthesis method for a hybrid sulfide catalyst featuring surfactant-intercalated tin(IV) disulfide (SnS2) nanosheets heterojuncted with bismuth(III) sulfide (Bi2S3) needles. The surfactant hexadecyltrimethylammonium bromide (CTAB) plays a vital role in transforming the morphology of the components and the formation of their heterojunction. The resulting catalyst exhibits outstanding performance in reducing CO2 to formate, demonstrating the high formate Faradaic efficiency (FE) of over 90 % across a wide potential range from-0.8 to-1.3 V (vs. reversible hydrogen electrode (RHE)) and achieving a maximum FEformate of 97.2 % at-1.1 V (vs. RHE). In contrast, the partial current density of formate reaches about 350 mA cm- 2 at-1.35 V (vs. RHE) in the flow cell. Furthermore, the catalyst demonstrated exceptional stability, with a high selectivity towards formate production maintained at a current density of 156 mA cm- 2. Theoretical calculations and in situ Raman indicate that the SnS2/Bi2S3 heterojunction active sites optimize the free energy for the *H and *OCHO intermediates, thereby facilitating the formation and desorption steps of *HCOOH, ultimately leading to formate yield efficiently. Our investigation offers a strategic method and valuable insights for designing catalytic materials with rich interfaces for efficient CO2 reduction reactions.

Injecting CO2 into deep coal seam is recognized as a promising strategy for carbon sequestration and enhancing coalbed methane recovery (CO2-ECBM). For high-temperature and high-pressures reservoirs conditions, CO2 typically exists in a supercritical state (ScCO2), and its influence on the adsorption mechanism of coal is not yet fully understood. To address this concern, a comprehensive study including N2-CH4 and ScCO2-CH4 displacement tests, as well as ScCO2 and CH4 adsorption tests, combined with various microscopic characterization methods, was conducted. Additionally, Density functional theory (DFT) calculations were utilized to determine the adsorption energies of different molecules in anthracite after exposure to ScCO2. The findings revealed that the isothermal adsorption of ScCO2 in anthracite exhibited a non-monotonic trend, with the lowest adsorption capacity occurring near the critical phase. The pyrrole-N site has a stronger adsorption to CO2 than to CH4 and N2. Comparatively, pyridine-N site is less favourable for CO2 adsorption. The alternation of nitrogen configurations could effectively enhance the CO2 adsorption capacity, and potentially facilitate the release of CH4 from the coal matrix. This correlation between experimental observations and theoretical calculations offers profound insights into the mechanisms of CO2 geological storage and the potential for methane extraction.

Hard carbon (HC) materials, with their abundant defect sites, expanded interlayer spacing and tunable porosity, have emerged as promise candidates for sodium-ion battery (SIB) anodes by optimizing distinctive sodium-ion adsorption/desorption and insertion/deintercalation behaviors. However, achieving precise pore structure regulation remains a critical challenge to overcome limitations in capacity and initial Coulombic efficiency (ICE). In this study, a novel inverse strategy-localized HC coating on a soft carbon (SC) matrix is presented to synergistically combine the merits of their distinctive porosity characteristics, contrasting conventional SC-coated HC designs. Employing phenolic resin and petroleum coke as HC and SC precursors, respectively, a HC-coated SC composite is successfully synthesized through ball milling and calcination. Comprehensive structural and electrochemical analysis reveals that the localized HC layer effectively regulates the pore structure of underlying SC matrix, enhancing sodium-ion storage capacity and ICE. Notably, by rationally adjusting the mass ratio of HC/SC precursors, the optimized composite anode delivers a reversible capacity of 342.5 mAh/g and an ICE of 78.8 % at a current density of 30 mA/g. These results significantly outperform the pure HC or SC anodes prepared under the same conditions. This study provides a new pore-engineering approach for designing high-performance hard-soft carbon anode composites for SIB.

At extremely low temperatures, the incorporation of zwitterionic polymers in constructing high-speed ion channels hold immense potential to exponentially enhance ionic conductivity, which is lethally compromised by solidification and increased viscosity of electrolytes. However, the network structure formed by zwitterionic groups is susceptible to disruption caused by cations and anions in the electrolyte, thereby affecting its structural stability and mechanical properties. In this study, high-concentration divalent cations were successfully employed as both antifreeze agents and cross-linkers to fabricate stretchable and low temperature resistant hydrogel electrolytes. This dual-role mechanism of different high-concentration divalent cations (M2+) in zwitterionic hydrogels was explicitly elucidated at the molecular level through the utilization of ex-situ Raman spectroscopy. This analysis has emphasized their crucial involvement in the formation of [-SO3- -M2+-SO3- -] coordination bonds with negatively charged groups (- SO3- ), thereby providing additional cross-linking points, as well as their hydration interactions with free water molecules, which contribute to its exceptional low temperature resistance. With the ion channels constructed from zwitterionic polymers and the low-temperature resistance given by the high salt concentration, the hydrogel electrolyte containing Ca2+ achieved an impressive low-temperature ionic conductivity of 5.9 mS cm-1, even at -50 degrees C. The assembled supercapacitors (SCs) demonstrated a remarkable areal specific capacitance of 100.8 mF cm- 2 at -40 degrees C, with a capacitance retention rate of 108.8 % after 10,000 cycles. This performance surpassed most reported antifreeze hydrogel electrolytes, offering valuable insights for designing flexible electrolytes with enhanced stability and high performance in low temperature environments.

Currently, MXene-based materials with room temperature sensing capabilities are emerging as candidates for next-generation gas sensors because of their exceptional sensitivity and selectivity. However, the commercialization of these sensitive materials is limited by their unsatisfactory response speed and humidity resistance. A straightforward lyophilization technique is developed to mitigate the adverse effects associated with the accordion-like layered structure of Ti3C2 MXene. This approach is further integrated with CeO2 nanocubes to increase the humidity resistance. As a result, the CeO2/few-layer Ti3C2 MXene composite exhibited markedly improves response speed, humidity resistance, and detection capabilities compared with its CeO2/multilayer Ti3C2 MXene counterpart. Specifically, the optimized composite demonstrates a rapid response time of 6.6 s, 85 % humidity resistance at 85 % relative humidity, a response value of 3.74 to 1 ppm NO2, and a detection limit as low as 10 ppb at room temperature. The performance of the CeO2/few-layer Ti3C2 MXene composite can cover most commercial NO2 gas sensors on the market with nearly ideal sensing behavior, facile fabrication, and room temperature working conditions. In addition, simple modification provides more opportunities for designing MXene-based gas sensors for various applications with different target gases at room temperature.

The development of high-performance, eco-friendly biochar electrodes for EDLCs holds significant potential for practical energy storage, yet their widespread application remains hindered by suboptimal electrochemical performance. To address both environmental concerns associated with conventional potassium hydroxide and performance limitations, we propose a novel strategy for synthesizing three-dimensional porous graphitized carbon from Semen Ziziphi Spinosae (SZS) biomass using potassium ferrioxalate as a dual-function activator. This approach simultaneously enables in-situ graphitization and activation, streamlining the synthesis process while eliminating reliance on conventional corrosive activators. The optimized SZS-derived activated carbon (SZAC-3) exhibits a hierarchical porosity with an ultrahigh specific surface area of 912.95 m2 & sdot;g- 1, facilitating rapid ion transport and charge storage. Electrochemical evaluations demonstrate exceptional performance of a high specific capacitance of 215 F g- 1 at 0.5 A g- 1 and outstanding cycling stability with 96.15 % capacity retention after 5000 cycles at 20 A g-1. The assembled symmetrical coin-like supercapacitor delivers a competitive energy density of 9.44 Wh kg- 1 and power density of 250 W kg-1, highlighting significant potential for practical applications. This study verifies that SZS is a sustainable carbon precursor, while demonstrating K3[Fe(C2O4)3] as an effective eco-friendly activator alternative to potassium hydroxide, resulting in a more cost-effective production of high-efficiency supercapacitor electrode material.

Tin-based anodic materials, benefiting from their large theoretical specific capacity and minimal operating potential, are considered high-development potential alternative anodes for lithium-ion batteries (LIBs). Nevertheless, the alloying-dealloying processes between tin (Sn) and lithium ions result in severe volume expansion, which leads to a poorly stabilized solid-electrolyte interface (SEI) layer and resultant inferior cycling performance, posing major obstacles to their commercialization. Herein, a structural regulation strategy was proposed to optimize the interstitial void buffer layer within yolk-shell structures to mitigate the lithiation-associated volume expansion. The tetraethyl orthosilicate-hydrolyzed SiO2 layer was located between Sn and the resin-derived carbon coating, whose thickness could be sophisticatedly optimized via regulating the hydrolysis durations. Following the carbonization and etching, an optimized buffer layer was encapsulated within a protective carbon shell (Sn@Void@C), which could effectively accommodate Sn's volume expansion during the alloying period, significantly enhancing its performance in electrochemical processes and structural stability. Specifically, the Sn@Void@C anode retained a high specific capacity of 720 mAh g-1 after 400 cycles at 0.2 C and demonstrated an outstanding capacity of 520 mAh g-1 after 500 cycles at 0.5 C. This work provides a facile and effective strategy for rationally designing tin-based anodes for lithium-ion batteries.

Sn-based materials are among the most promising catalysts for CO2 reduction reaction (CO2RR) to formic acid. However, the complex electrochemistry-induced surface reconstruction under negative potentials has hindered the precise elucidation of the structure-performance relationship. Herein, machine learning potential (MLP) is employed to accelerate molecular dynamics (MD) simulations, and pH-field coupled microkinetic modelling is perfromed to unravel the pH dependence of CO2RR at the reversible hydrogen electrode (RHE) scale. Encouragingly, the developed MLP reveals that SnO2 adopts a nanorod-like morphology, accurately reproducing experimentally observed reconstruction phenomena. Additionally, SnS2 prefers to form a rougher surface. Leveraging the precisely determined reconstructed surface, the exciting pH-dependent behavior of Sn-based catalysts is highlighted: the increase of pH will cause a left-shift in the CO2RR volcano and ultimately enhance the catalyst's activity. Most importantly, the excellent agreement between the theoretical simulations and our subsequent experimental measurements validates the accuracy of the simulations in terms of turnover frequencies, providing a clear benchmarking analysis between experiments and the MLP-MD-assisted pH-field coupled microkinetic modelling. This work not only offers a valuable MLP-based approach for studying surface reconstructions, but also provides new guidance for the design of high-performance complex catalysts for CO2RR.

The electrode/electrolyte interfacial depletion layer could accelerate the carriers' separation along their diffusion pathway via induced internal electric field (IEFs). Enhancing the proportion of depletion layer and shortening carriers' diffusion length (L) are crucial for developing hematite (alpha-Fe2O3) base catalysts with high carrier utilization efficiency, yet remains challenging. Herein, a sulfur and nitrogen co-pyrolyzed strategy is proposed to simultaneously modulate the electronic depletion layer and microstructural diffusion layer in anodized iron oxides nanotubes (SN co-pyrolyzed NTs). The nanowalls of anodized NTs were deliberately thinned as smaller than the diffusion length of carriers within hematite, resulting in ternary Fe2O3/Fe3O4/FeS heterostructure with optimized depletion layer width (W) and surface potentials. An optimal W (similar to 3.35 nm) to L (similar to 3.18 nm) ratio was achieved as larger than 1, indicating an overlapped electronic depletion layer and microstructural diffusion layer was constructed. This optimal W/L ratio implies that the carriers' diffusion process would be fully accelerated via the IEFs, which could massively promote the carriers' separation and subsequent utilization efficiency. The SN co-pyrolyzed photoanode exhibited significant improved onset potential of 0.62 V-RHE, state-of-the-art photocurrent density of 22.6 mA cm(-2) (1.23 V-RHE) and incident photon-to-current conversion efficiency of 65 %, which surpass ever reported hematite based photoanodes. DFT calculations proves that the induced electron-deficient surface could create favorable adsorption sites for oppositely charged intermediates and reduce energy barrier of *OOH formation. This work provides a facile strategy for manipulating the carrier kinetics via microstructural and electronic optimization and is expected to facilitate the design of new photoelectrodes for solar-to-fuel energy conversion.

Although silicon (Si) is widely recognized as one of the most promising anode materials for next-generation lithium-ion batteries (LIBs), its severe volume expansion and poor electrical conductivity pose significant challenges for commercialization. To address these challenges, a mesoporous carbon shell encapsulated silicon/ graphite composite (Si/G@PCS) with distinctive two-dimensional conductive network and self-adaptive internal spacing was deliberately designed in this work. Silicon nanoparticles (Si NPs) were uniformly dispersed on graphite sheets through ball milling to create a highly efficient conductive network, which were further entirely encapsulated by a nanoporous carbon shell via pyrolysis, forming a capsule-like core-shell structure. The integration of assembled graphite nanosheets featuring abundant internal voids spacing could significantly improve the electrical conductivity of Si NPs while effectively mitigate the lithiation associated volume expansion. Moreover, the abundant mesopores on the outer carbon shell provided rapid ion transport pathways, thereby enhancing the anode's overall electrochemical performance. The prepared Si/G@PCS electrode exhibited a high initial coulombic efficiency (ICE) of 80.65 % during the first cycle. After 100 cycles at a current density of 0.2 A g-1, the electrode retained a reversible capacity of up to 971.5 mAh g-1. Notably, even at a higher current density of 2 A g-1, it still delivered a capacity of 711.5 mAh g-1. The rational design and preparation for Si/ G@PCS composite proposed in this study provides a feasible strategy for the large-scale preparation of highenergy-density silicon anode materials.