The electrochemical CO₂ reduction reaction (CO₂RR) holds great promise for closing the anthropogenic carbon cycle, yet conventional aqueous electrolytes epitomized by KHCO₃ suffer from intrinsically low CO₂ solubility, sluggish mass transport, and poor product selectivity, which collectively hamper catalytic efficiency and pathway controllability. Here, we report a rationally designed hybrid electrolyte system comprising 1-ethyl-3-methylimidazolium chloride ([EMIM]Cl) supplemented with KHCO₃, integrated with composition-tunable CoZn oxide nanoflower catalysts, that enables highly efficient and precisely switchable conversion of CO₂ to either CO or formic acid (HCOOH). Through an integrated approach combining electrochemical measurements, in situ infrared spectroscopy, and multiscale theoretical simulations (density functional theory + ab initio molecular dynamics), we uncover a previously unrecognized cooperative proton tunneling mechanism: water molecules act as proton-bridging mediators, constructing a linear [EMIM]-H···O-H···O-C(O)^- pre-reaction complex at the electrode interface that dramatically lowers the activation barrier of the proton-coupled electron transfer step. Critically, the Co:Zn ratio dictates the electronic structure of active sites; Co centers stabilize *COOH intermediates for CO evolution, whereas Zn centers favor *OCHO stabilization for HCOOH formation. Under optimized conditions, the Co:Zn = 2:1 catalyst achieves a Faradaic efficiency of 80.4% for CO, whereas the Co:Zn = 1:2 counterpart delivers 70.9% for HCOOH. This work establishes a paradigm of “proton tunneling channel engineering” via electrolyte-catalyst synergy, offering a molecular-level blueprint for precise control over multi-electron electrochemical transformations beyond CO₂RR.

Solid polymer electrolytes (SPEs) are regarded as ideal solid electrolytes for next-generation lithium-ion batteries due to their high safety, but their low ionic conductivity limits practical applications. The incorporation of garnet-type Lithium Lanthanum Zirconium Oxide (LLZO)-based electrolytes with high Li⁺ conductivity is an effective strategy to enhance the performance of polyethylene oxide (PEO)-based SPEs. In this study, highly Li⁺-conductive Ga-doped LLZO (Li_6.4Ga_0.2La₃Zr₂O₁₂) was prepared by wet and dry methods, yielding samples denoted as wet-LLZO and dry-LLZO, with abundant and minimal surface residual alkali, respectively. These LLZO nanoparticles with different residual alkali were incorporated as fillers in composite solid polymer electrolytes (CSPEs). Studies demonstrate that the residual alkali, such as Li₂CO₃, on the LLZO surface effectively disrupts the ordered arrangement of PEO segments, significantly reducing their crystallinity and thus facilitating Li⁺ transport. Based on this, CSPE with 15 wt% wet-LLZO achieves a high ionic conductivity of 0.80 mS cm^-1 and a lithium-ion transference number of 0.36 at 60 °C. The assembled Li/LiFePO₄ all-solid-state battery maintains a discharge specific capacity of 142.5 mAh g^-1 and a Coulombic efficiency exceeding 99% after 300 cycles at a 1.0 C rate. This work reveals the role of residual surface alkali in the LLZO composite solid electrolyte, providing novel insights for designing high-performance solid-state batteries through filler surface engineering.

Layered transition metal oxide (LTMO)-based sodium-ion batteries (SIBs) are prime candidates for outdoor stationary energy storage systems; however, their application is limited by rapid capacity decay under high-rate and elevated-temperature conditions. Herein, we propose a synergistic electrolyte engineering strategy based on a binary solvent system comprising propylene carbonate (PC) and ethyl methyl carbonate (EMC), supplemented with the film-forming electrolyte additives fluoroethylene carbonate (FEC) and vinylene carbonate (VC). The mixed electrolyte has been shown to enable the in situ formation of chemically stable, thermally resistant, and mechanically robust films on the LTMO cathode. The distinct functional roles of VC, FEC, PC, and EMC are systematically elucidated. Consequently, this synergistic electrolyte strategy enables LTMO-based SIBs to achieve outstanding cycle stability at high rates and elevated temperatures. Specifically, the LTMO-based SIBs delivered an initial capacity of 80 mAh g^-1 at 10 C (from the long-term cycling test), retained 62.7 mAh g^-1 after 600 cycles at 10 C, and retained 54.8 mAh g^-1 after 300 cycles at 1 C at 90 °C. This study presents a scalable strategy for developing high-stability LTMO-based SIBs with strong adaptability to aggressive outdoor stationary energy storage environments.

Converting discarded polyolefin separators into valuable carbon nanotubes (CNTs) not only contributes to the high-value utilization of discarded separators, but also offers a green approach to construct advanced CNT-based generators. However, the controlled carbonization of discarded polyolefin separators into high-quality CNTs remains challenging, and the mechanism of electricity generation in CNTs remains obscure. Herein, we report the “all-in-one” catalytic strategy using multi-component Ni/Mo/Mg catalysts to realize the controllable carbonization of discarded polyolefin separators into high-quality CNTs. By adding Mo and Mg to Ni in a molar ratio of 5/0.1/0.5 (Ni/Mo/Mg), the catalyst displays high catalytic activity, dispersion, and stability, and achieves a CNT yield of 57.4 wt%. Thanks to the good photothermal conversion capability and excellent wettability, the CNT evaporator achieves an evaporation rate of 2.73 kg m^-2 h^-1, a photo-to-thermal efficiency of 95.4%, and an open-circuit voltage of 0.221 V under laboratory conditions, which ranks as one of the most efficient evaporators/generators. In practical experiments, the total water production and voltage output are 2.51 kg m^-2 over 5 h and 0.215-0.265 V, respectively. Molecular dynamics simulation results show that the surface functional groups interact more strongly with H⁺ than with OH^-. With the continuous evaporation of bulk water, H⁺ moves faster upward along the nanochannel than OH^-, thus forming a potential difference. This study provides an eco-friendly route for synthesizing advanced carbon nanomaterials and co-generating freshwater and electricity.

Coal is a low-cost, carbon-rich feedstock for preparing hard carbon (HC) anodes, making coal-derived carbon attractive for sodium-ion battery applications. However, direct carbonization of coal usually involves softening, aromatization, and molecular rearrangement, which promote the ordered growth of graphitic microcrystals with limited interlayer spacing and insufficient nanopores, thereby restricting sodium-storage capacity. To address this issue, we introduce a chitosan/glutaraldehyde (CS/GA)-assisted molecular-network regulation strategy to tailor both the carbon framework and surface chemistry of coal-derived HC. CS is first immobilized on oxidized coal (OC) through hydrogen bonding and electrostatic interactions and then cross-linked with GA via a Schiff-base reaction, forming a molecular network that suppresses the ordered growth of graphitic microcrystals during carbonization. Meanwhile, chitosan serves as an endogenous nitrogen source, enabling in situ nitrogen doping. The optimized SGHC-8 (CS/GA-cross-linked coal-derived HC) exhibits expanded interlayer spacing, increased defect density, and abundant nanopores, which contribute to enhanced sodium storage, especially in the low-voltage plateau region. As an anode for sodium-ion batteries, SGHC-8 delivers a reversible capacity of 350.5 mAh g^-1, an initial coulombic efficiency of 80.6%, and a plateau capacity contribution of 48.5%. Combined kinetic and structural evidence reveals that Na⁺ storage in SGHC-8 proceeds through sequential adsorption, interlayer insertion, and nanopore filling. This work provides a feasible strategy for converting coal into high-performance HC anodes through cross-linking-induced microstructure regulation.

Thermal intensification of CO₂ electroreduction to the key feedstock formate is thermodynamically favorable; however, its practical utility is often compromised by solubility-driven CO₂ depletion and parasitic hydrogen evolution. Here, we develop a solid-liquid-gas triphase boundary (TPB) to circumvent this limitation. This architecture decouples the CO₂ supply from bulk solubility constraints, ensuring reactant availability under thermal activation. Electrochemical evaluation demonstrates that the TPB electrode maintains a Faradaic efficiency exceeding 80% at high temperature, along with a significant increase in formate production rate. Kinetic analyses reveal a distinct mechanistic divergence, showing that the TPB enhances turnover frequency (TOF) by 36% at 50 °C relative to 20 °C, whereas the conventional biphasic system suffers a 70% TOF decline. Mechanistic simulations indicate that the TPB sustains near-saturated interfacial CO₂ concentrations while facilitating rapid formate expulsion at elevated temperatures, thereby preventing product accumulation. This work presents a viable strategy for thermally intensified electrocatalysis by integrating material superhydrophobicity with thermal kinetics.

Planar inverted water-based perovskite solar cells (PIW-PSCs) can be fabricated without toxic organic solvents. However, in the aqueous deposition route, organic ammonium salts (OAS) must penetrate the precursor film while simultaneously driving phase conversion. This deposition method results in slow and nonuniform conversion. Here, urea is used as a water-compatible additive that improves precursor wetting and promotes further development of the internal porous structure by the subsequent thermal treatment. The resulting porous precursor provides more accessible transport pathways for OAS, thereby promoting more complete conversion of Pb(NO₃)₂ into perovskite. Consequently, the resulting perovskite film exhibits enlarged grains, reduced defect density, and reduced residual compressive stress. The corresponding PIW-PSC achieves a champion power conversion efficiency (PCE) of 20.39%, while the PIW-PSC device shows stable power output for 20 min at a fixed bias corresponding to its maximum-power-point voltage. Unencapsulated PUS-L devices retain 84% of their initial PCE after approximately 1,000 h of ambient storage (30%-35% relative humidity, ~25 °C) and 68% after 450 h of thermal aging at 80 °C under N₂. This strategy combines the water compatibility, Pb²⁺ coordination, and thermally induced transformation of urea to regulate precursor-film morphology and facilitate OAS transport during the nitrate-to-halide conversion of Pb(NO₃)₂ precursors.

Tributyl phosphate (TBP) is regarded as a potential solvent for elevated temperature lithium metal batteries due to its high boiling point, low vapor pressure and excellent thermal stability. However, the strong interaction between the polar P=O groups of phosphate and Li⁺ slows down Li⁺ kinetics, and the vigorous reductive decomposition of phosphate ester compounds on the anode leads to an unstable and fragile solid electrolyte interphase (SEI), resulting in poor cycling stability at elevated temperatures. Herein, an electrolyte system that employs functionalized ethoxylated (pentafluoro)cyclotriphosphazene (PFPN) and TBP establishes a dipole/pseudo-hydrogen bond synergistic solvation relationship to resolve the strong coordination between TBP and Li⁺ and the resulting SEI instability. Specifically, the synergistic dipole-dipole interactions between the N-P ring (δ⁺P) of PFPN and the P=O group (δ^-O) of TBP, combined with pseudo-hydrogen bonds between δ^-F of PFPN and δ⁺H of TBP alkyl chains, generate a drag effect that weakens Li⁺-TBP coordination, thereby enhancing Li⁺ transport kinetics. Moreover, the low lowest unoccupied molecular orbital level of PFPN enables its preferential decomposition on the anode, which cooperates with the FSI^--rich inner solvation sheath to construct a robust =P-N/LiF-rich SEI and cathode electrolyte interphase (CEI), effectively suppressing side reactions between TBP and the Li metal anode. Consequently, the NCM811||Li cells using the electrolytes deliver outstanding rate capability and stable long-term cycling at 60 °C. In addition, the Ah-level Li||NCM811 pouch cell shows excellent safety, characterized by no ignition upon nail penetration at full charge and a high thermal runaway onset of 224 °C from accelerating rate calorimetry testing.

Aqueous rechargeable batteries are promising for large-scale energy storage, but MnO₂ electrodes suffer from manganese dissolution and Jahn-Teller-related instability. Here, we investigate sulfate-anion-involved charge storage in layered δ-MnO₂ symmetric cells. Ex situ spectroscopy, thermal analysis, and elemental mapping show state-dependent sulfur signals accompanied by Mn valence evolution and modest, partially reversible local coordination changes. First-principles calculations indicate that sulfate accommodation and migration within a modeled interlayer are energetically plausible. These results support sulfate-coupled charge compensation and suggest possible interlayer accommodation, while surface adsorption, near-surface storage, and electrolyte trapping cannot be excluded under the present ex situ conditions. The MnO₂ electrode delivers 154.2 mAh g^-1 at 0.2 A g^-1, and the symmetric cell achieves 107.94 Wh kg^-1 at 180 W kg^-1 with 93.7% capacity retention after 3,000 cycles. This work provides evidence for sulfate-coupled charge compensation in layered MnO₂.

Despite their power conversion efficiencies reaching 28.0%, formamidinium lead iodide (FAPbI₃)-based perovskite solar cells (PSCs) suffer from moisture-induced phase degradation that initiates preferentially at the SnO₂/FAPbI₃ buried interface, yet the coupling between humidity exposure and thermal stress at the interface remains unclear. Here, we introduce a CsCl interlayer at the buried interface of n-i-p-structured PSCs and examine its role in reinforcing the structural resilience of FAPbI₃ against moisture at elevated temperature. This interfacial role is distinguished from the improved crystallinity of the pristine FAPbI₃ film that CsCl is already known to provide. The CsCl interlayer blocked the irreversible formation of Pb-O-related species and enabled partial reconversion of the moisture-driven δ-phase and PbI₂ back to the α-phase during post-exposure annealing. Sequential changes in the lattice bonding environment across the pristine, humidity-exposed, and post-exposure annealed films were analyzed by complementary X-ray diffraction, grazing-incidence X-ray diffraction, Fourier-transform infrared spectroscopy, and X-ray photoelectron spectroscopy to elucidate the CsCl interlayer-induced stabilization mechanism in FAPbI₃.

Dielectric barrier discharge (DBD) plasma-coupled photocatalysis offers a promising route for CO₂-to-syngas conversion, but rational optimization remains challenging because operating variables are strongly coupled. Here, we develop a small-sample machine-learning framework to predict and optimize a plasma-coupled photocatalytic CO₂ conversion system using a Cu-Pd/TiO₂ photocatalyst. Using 120 experimental runs, five operating parameters, including discharge power, catalyst dosage, gas flow rate, relative humidity, and light intensity, were evaluated against CO₂ conversion, CO yield, and H₂ yield. Among the evaluated models, a shared-weight Gradient Boosting Regressor (GBR)-Kernel Ridge Regression (KRR) hybrid model achieved the great predictive performance, with test-set R² values of 0.947, 0.950, and 0.954 for CO₂ conversion, CO yield, and H₂ yield, respectively. Permutation importance and SHapley Additive exPlanations (SHAP) analyses identified relative humidity, light intensity, and discharge power as the most influential variables and revealed distinct model-predicted trends across the three outputs. The trained model was further used for constrained optimization under target H₂/CO ratios of 1 and 2, followed by experimental validation of the selected operating conditions. Overall, this work establishes a data-driven strategy for interpreting nonlinear plasma-photocatalytic CO₂ conversion and provides practical guidance for syngas-ratio regulation under experimentally relevant conditions.

Developing hydrogen evolution reaction (HER) electrocatalysts that combine high activity with reliable operation in different electrolytes remains important for clean-hydrogen and electrochemical-energy technologies. In this study, CoRu composite oxides with adjustable Co/Ru molar ratios were formed in situ on nickel foam through co-precipitation and subsequent high-temperature calcination, and their HER behavior was examined in alkaline, neutral, and near-neutral media. Co₄Ru₁O_x showed the good activity and durability. In 1 M KOH, current densities of 100, 300, and 700 mA cm^-2 were obtained at overpotentials of 78, 127, and 196 mV, respectively; the corresponding Tafel slope was 21.64 mV dec^-1. The electrode also operated for 200 h in both 1 and 6 M KOH. When incorporated into a membrane electrode assembly electrolyzer, Co₄Ru₁O_x||NF sustained overall water splitting at 100 mA cm^-2 for 200 h. In 1 M phosphate buffer solution, only 16 mV was needed to deliver 10 mA cm^-2, and stable operation was again maintained for 200 h. High-current HER activity was also obtained in saturated KHCO₃, while a Zn-CO₂ cell using this catalyst reached a maximum power density of 9.6 mW cm^-2. Collectively, these findings identify Co₄Ru₁O_x as a multifunctional HER electrode suited to several electrochemical environments.

The use of nonaqueous electrolyte in manganese-ion batteries (MIBs) has attracted increasing scientific attention because of their unique properties. These systems significantly reduce water-molecule interference in electrode reactions, effectively precluding unwanted side reactions such as the hydrogen evolution reaction, which commonly occurs in aqueous electrolytes. Nonaqueous electrolyte development is still a challenge, though. Mn²⁺ has a high charge density, which leads to sluggish Mn²⁺ kinetics and greatly limits the development of nonaqueous MIBs. In this study, BiCl₃ is used as an electrolyte additive to enhance the reaction kinetics of Mn²⁺ in a diglyme-based nonaqueous electrolyte. Electrochemical testing shows that the polarization voltage of Mn||Mn symmetric cells is greatly reduced following the addition of BiCl₃. Full characterization by X-ray diffraction and scanning electron microscopy, combined with density functional theory calculations, suggests that Bi³⁺ undergoes a spontaneous galvanic replacement reaction with the Mn anode. This process enables the in situ formation of a Bi-containing interphase, which helps reduce the activation barrier for charge transfer. Thus, the full cell with a Cu_1.8S cathode delivered an improved average discharge capacity of 166.1 mAh g^-1 over 200 cycles at 100 mA g^-1. This work provides perspectives for designing the interfacial chemistry of MIBs.

Syngas-derived higher alcohols (C₂₊OH) are vital clean fuels under dual-carbon targets, yet inherent catalytic bottlenecks hinder industrialization. This review systematically correlates core defects across five mainstream catalyst families with targeted modification strategies and structure-selectivity rules. Cu-Co catalysts exhibit overly broad product distribution and phase segregation; La/Mn doping and plasma activation accelerate C-C coupling. Cu-Fe catalysts sinter easily and undergo phase separation; Mg/K/Ce doping and carrier tuning reinforce bimetallic interfacial synergy. Modified Cu methanol catalysts lack stable active sites; particle size control, pH adjustment, and ammonia evaporation enrich Cu-ZnO_x interfaces. Mo catalysts resist sulfur and carbon deposition but require harsh reaction conditions; K/La doping and porous carbon carriers improve long-chain alcohol selectivity. Rh catalysts exhibit excellent C₂₊OH selectivity but incur high noble-metal costs; single-atom immobilization reduces Rh consumption. Multifunctional tandem catalysts balance activity and selectivity via matched dual active sites. This study establishes a “bottleneck-modification” matching system, offering theoretical support for low-cost high-performance catalysts and industrial syngas-to-higher-alcohol technology.

Hydrogen production via catalytic decomposition of methane (CDM) offers a CO₂-free route for simultaneous hydrogen and solid carbon generation. However, practical implementation remains limited by catalyst deactivation, metal contamination in the carbon product, and inefficient post-reaction purification. In this work, Ni-promoted (La_0.75Ca_0.25)(Cr_0.5Mn_0.5)O_3-δ (Ni-LCCM) perovskite catalysts prepared via a nitrate-based route were evaluated for CDM. Under thermal CDM at 750 °C without pre-reduction, 050Ni-LCCM achieved a Ni-normalized carbon productivity of up to 11.53 g_C·g_Ni^-1. A non-monotonic dependence of intrinsic carbon productivity on Ni loading was observed, with local maxima for 050Ni-LCCM and 150Ni-LCCM. These two experimental compositions were represented by the 2Ni-LCCM and 6Ni-LCCM models in the density functional theory (DFT) calculations. The 2Ni-LCCM and 6Ni-LCCM models showed lower relative rate-limiting activation barriers than those of neighboring configurations. Together with structural characterization, these results suggest that methane decomposition activity is strongly influenced by local Ni configuration, Ni reducibility, and site accessibility rather than by total Ni loading alone. Carbon characterization showed the formation of predominantly nanocrystalline graphitic carbon, including mixed carbon nanostructures such as carbon nanotubes, carbon nanofibers, and carbon nano-onions. Post-reaction purification using 5 M HNO₃ reduced the residual inorganic content to 4.20% and 1.41% for carbon products from 050Ni-LCCM and 150Ni-LCCM, respectively, corresponding to thermogravimetric analysis (TGA)-based carbon contents of approximately 95.8% and 98.6%. Overall, the results demonstrate that Ni-LCCM is an effective catalyst system for CDM, in which composition-dependent Ni configurations influence intrinsic carbon productivity while enabling recovery of high-carbon-content solid products after mild acid treatment.

Yb³⁺-doped perovskite nanocrystals (NCs) featuring quantum-cutting capability exhibit enormous potential for luminescent solar concentrators (LSCs) due to their theoretically achievable 200% photoluminescence quantum yield (PLQY). However, their practical applications are still limited by defect-assisted nonradiative recombination, insufficient exciton-to-Yb³⁺ energy transfer efficiency, and poor operational stability. Herein, we demonstrate a CdCl₂ post-treatment strategy to regulate the lattice structure and photoluminescence (PL) dynamics of Yb³⁺:CsPbCl₃ NCs. As a result, the PLQY is significantly enhanced from 125.3% to 177.4%, accompanied by an increase in exciton to Yb³⁺ energy transfer efficiency from 75.9% to 86.4%. In addition, the treated NCs exhibit substantially improved photostability and thermal stability, with the thermal activation energy increasing from 61.8 ± 6.2 to 90.9 ± 2.4 meV. Compared with ZnCl₂, NiCl₂, and CuCl₂ treatments, CdCl₂ shows uniquely superior enhancement of the exciton to Yb³⁺ energy transfer efficiency and Yb³⁺ emission. Flexible LSCs fabricated based on the treated NCs exhibit high visible transparency and efficient near-infrared (NIR) photon waveguiding and concentrating capability, achieving an internal optical efficiency exceeding 120% and delivering enhanced photovoltaic performance when coupled with silicon solar cells. This work provides an effective strategy for developing high-performance Yb³⁺-doped perovskite NCs and flexible transparent LSCs for building-integrated photovoltaics.

Sodium chloride (NaCl) is attractive as a solid electrolyte because of its wide electrochemical stability window, excellent dry-air stability, favorable cathode compatibility, and low cost; however, its intrinsically low ionic conductivity has severely limited practical application. Here, we report an Al³⁺/O^2- co-doping strategy that introduces Na⁺ vacancies and mixed Cl^-/O^2- anion environments into the NaCl lattice, thereby converting NaCl from a poor ionic conductor into a fast-ion-conducting solid electrolyte. The optimized composition, Na_0.4625Al_0.25Cl_0.7875O_0.2125, exhibits an ionic conductivity of 2.7 × 10^-4 S cm^-1 at 30 °C. Through combined X-ray diffraction, solid-state nuclear magnetic resonance, and pair distribution function analysis, Na_0.4625Al_0.25Cl_0.7875O_0.2125 is identified as a single-phase face-centered cubic structure (space group Fm-3m) that hosts a high concentration of Na⁺ vacancies (37.6%) at the 4a sites, creating a continuous 3D transmission network for rapid Na⁺ migration. Electrochemically, Na_0.4625Al_0.25Cl_0.7875O_0.2125 exhibits a wide stability window of 1.05~4.24 V vs. Na₂Sn. In an all-solid-state cell with the configuration NaNi_1/3Mn_1/3Ti_1/3O₂||Na_0.4625Al_0.25Cl_0.7875O_0.2125||Na₃PS₄||Na₂Sn, capacity retentions of 89% and 83% are achieved after 100 cycles over voltage windows of 2.4-4.2 and 2.4-4.4 V, respectively.

Electrical double layers (EDLs) constitute fundamental electrochemical interfaces that, when dynamically regulated, enable tight coupling between energy transduction and information processing. Recent advances have progressively shifted the role of EDLs from passive, equilibrium charge-screening structures to actively reconfigurable ionic-electronic interfaces, thereby establishing a unified physicochemical framework for solid-liquid triboelectricity, triboiontronics, and the emerging iontrovoltaic effect. Here, we synthesize a dynamic EDL-centered perspective that connects the evolution of EDL theory with recent developments in iontronic systems. This framework outlines a continuous conceptual progression from classical conductive-interface descriptions and the two-step model of non-conductive interfaces to triboiontronic regimes in which mechanically induced charge separation drives dynamic ion polarization and further to semiconductor-liquid interfaces where EDL modulation couples with space charge regions to give rise to the iontrovoltaic effect. In parallel, device architectures evolve from solid-liquid triboelectric nanogenerators to triboiontronic nanogenerators and ultimately to iontrovoltaic nanogenerators, reflecting increasing integration of ionic dynamics with electronic transport. Across these regimes, the functional role of EDLs expands from static charge screening to dynamic electrostatic induction, directional ionic transport, and coupled ionic-electronic modulation. This evolution establishes dynamic EDLs as a general platform for co-regulating energy flow and information flow across solid-liquid interfaces. More broadly, dynamic EDLs provide a unifying ionic framework that links interfacial energy conversion with information processing, offering a physical basis for the development of bioinspired iontronic systems and embodied intelligence.

NaFePO₄ (NFP) is a promising alternative to LiFePO₄, offering advantages such as the abundance of natural sodium resources. However, its common crystal phase, maricite, is typically electrochemically inert. This study presents a novel, synthesis-controllable, and rechargeable maricite NFP cathode material, specifically Na_0.33Fe_0.95Ca_0.06PO₄, for sodium-ion batteries. The structure provides two main benefits: Ca²⁺ doping broadens the bulk sodium-ion transport channels, while the dynamic and persistent Jahn-Teller distortion caused by the coexistence of Fe⁴⁺, Fe³⁺, and Fe²⁺ induces internal lattice distortion, effectively activating its electrochemical activity. Additionally, nanocrystallization introduces external structural disorder, further shortening the ion diffusion path. This cathode exhibits a high reversible capacity of 178.6 mAh g^-1 at 50 mA g^-1 and a material-based energy density of 415 Wh kg^-1. This study offers a general strategy for activating electrochemically inert yet potentially viable battery materials, providing new insights for developing next-generation, high-performance, and low-cost energy storage systems.

NiFe hydroxide has emerged as a highly promising electrocatalyst in water electrolysis, yet its application in catalyzing the hydrogen evolution reaction (HER) remains challenging. Herein, we report a corrosion-reconstruction strategy to fabricate RuO₂ nanocluster-endowed NiFe hydroxide [RuO₂/NiFe(OH)_x] as an efficient electrocatalyst for HER application. Density functional theory (DFT) calculations provide insight into the HER mechanism, revealing that the reconstructed surface enriched with RuO₂ nanoclusters optimally adsorbs water molecules. This modification also induces a shift of the *H adsorption site from oxygen atoms to ruthenium atoms due to electron transfer effects, facilitating the desorption of *H and promoting efficient H₂ formation. The synthesized RuO₂/NiFe(OH)_xcatalyst delivers prominent HER activity (149 mV at 100 mA cm^-2) and robust operational stability in a water-splitting device, sustaining 200 mA cm^-2 for 100 h with almost no obvious voltage increment. Importantly, the fabrication of a large-area electrode demonstrates that this simple, room-temperature corrosion-reconstruction strategy is a promising and viable route for the application of HER electrocatalysts.