Selective CO₂ photoreduction via artificial photocatalysis into high-value chemical feedstocks such as CO is a productive strategy for remitting environmental problems and energy crises. Nevertheless, photocatalysts generally endure low activity and poor product selectivity due to the low light/CO₂ capture and slow dynamic transfer of photogenerated electrons. Herein, we describe an all-in-one lignin-based artificial thylakoid nanovesicle (AiO-L-ATN) using the confined growth strategy of lignin molecules, inspired by the chloroplast's photosynthesis mechanism. Such AiO-L-ATN possesses a high CO generation rate of 98.8 μmol g⁻¹ h⁻¹ at normalized active mass with a satisfactory selectivity of 92.1% in a gas-solid system with H₂O, exceeding 26 times that of the primary ZnCdS. Besides, introducing carbon nanovesicles significantly improves CO₂ capture performance, narrows the band gap, expands the wavelength range of light absorption, and accelerates the separation of photogenerated electrons. Density functional theory (DFT) calculation reveals that the carbon nanovesicles with various functional groups favor *CO₂ adsorption, *COOH production and conversion, as well as accelerate the dynamic transfer of photogenerated electrons, thereby endowing the outstanding CO₂ reduction rate and CO selectivity of AiO-L-ATN. This study not only provides valuable insights into the preparation of highly efficient photocatalysts but also offers novel avenues for CO₂ photoreduction.

Carbon-based substrates in Zn–MnO₂ flexible batteries have issues of low adhesion to MnO₂, impacting cycle stability and capacity performance. A triple-synergistic strategy integrating C–O–Mn covalent bonding, wettability optimization, and hierarchical mesoporous engineering via cellulose nanofibers/carbon nanotube (CNF/CNT)-modified carbon cloth (CC) was proposed. This design achieves a “surface-locking” effect between the substrate and electrode materials, which was proven through theory and experiments. Density functional theory (DFT) simulations validate the “surface-locking” mechanism, where oxygen functionalities on CNF can form robust CO–Mn bonds with MnO₂, inducing an increase in MnO₂ adsorption energy from −0.21 eV (pristine CC) to −1.36 eV, effectively suppressing Mn dissolution. Optimal wettability (contact angle: 97°) reduced Zn²⁺ desolvation and water-induced side reactions. Hierarchical pore structures accelerated Zn²⁺ diffusion. The optimized CC@CNF₁/CNT₂–MnO₂ cathode achieves 92% capacity retention after 2000 cycles at 1 A/g. This study highlights a surface engineering strategy that effectively addresses the individual challenges associated with interfacial adhesion, reaction kinetics, and ion transport. This strategy offers fundamental insights into electrode interface modification for the development of next-generation flexible energy storage systems.

Regulating the composition and valence states of layered O3-phase sodium-ion battery cathode materials can effectively mitigate issues related to complex phase transitions and poor air stability. However, further research is needed to optimize the controllable design of these structures and to better understand the transition mechanisms between different hierarchical phases. Herein, precise regulation of radial sodium-ion concentration, phase structure, and transition metal average valence of P/O cathode was realized through precursor-based secondary heterogeneous coprecipitation and solid-state sintering. Radial scanning transmission electron microscopy and electron energy loss spectroscopy characterization confirmed elemental migration during sintering, resulting in a gradient distribution of sodium content, phase structure, and transition metal valence states. This radially gradient continuous P2/O3–O3 composite without obvious phase interface reduces the barrier of sodium-ion transport at the phase interface to mitigates volume changes from O3–O3′ phase transitions, inhibits Na⁺/H⁺ exchange and acid erosion, and enhances moisture/carbon dioxide resistance, kinetic performance, and cycling stability. Consequently, after 10 h of exposure to 82% humidity and 3330 ppm CO₂ concentration, the first-cycle charge capacity of designed NM + 0.4 μm was 103.8 mAh g⁻¹, while the capacity loss reduced from 50.12% to 12.35%. This study presents a novel approach to enhancing the stability of layered cathode materials for sodium-ion batteries.

Metal chalcogenides represent promising anodes for sodium-ion batteries due to their high theoretical capacities and low material costs. However, their practical applications are hampered by inherently sluggish ion diffusion kinetics and severe volume expansion associated with their conventional conversion reaction mechanism. Here, we design a micro-nano ZnS/ZnSe heterostructured anode through in situ localized phase transformation strategy. This meticulously engineered architecture effectively modulates the Na⁺ storage mechanism from a typical conversion reaction to the surface redox pseudocapacitive reaction by precisely controlling the phase transition processes. Such structural control substantially increases Na⁺ diffusion sites and reconstructs internal electric fields. Moreover, abundant heterointerfaces and porous microstructure effectively alleviate internal mechanical stresses, provide a large number of Na⁺ storage sites and fast Na⁺ migration channels, collectively ensuring ultrafast reaction kinetics and superior structural stability of the ZnS/ZnSe. As a result, the ZnS/ZnSe exhibits a remarkable specific capacity of 796 mAh g⁻¹ at 0.1 A g⁻¹, stable cycling with no capacity decay over 1800 cycles at 15 A g⁻¹, and capacity retention of 89% even at ultrahigh current density of 20 A g⁻¹. Furthermore, the practical viability of this material is successfully demonstrated in a NaNi_1/3Fe_1/3Mn_1/3O₂(NFM)//ZnS/ZnSe full-cell, which shows outstanding cycling stability without noticeable capacity fading after 600 cycles.

The inherent hydroxide-rich (OH⁻) environment in alkaline media facilitates the two-electron oxygen reduction reaction (2e⁻ORR). However, the strong interaction between alkali metal cations and solvated water molecules significantly reduces the connectivity of the hydrogen bond network within the alkaline electric double layer, thereby severely impeding rapid proton transport at the electrode surface. Herein, we rationally designed ZnO with oxygen vacancies-driven [Fe(CN)₆]³⁻ coordination (denoted as Fe(CN)₆-ZnO-V_O) as an efficient 2e⁻ORR catalyst for H₂O₂ electrosynthesis. We demonstrate that the locally coordinated [Fe(CN)₆]³⁻ establishes pathways for rapid proton transfer at the electrode surface by forming a hydrogen bond network with interfacial water molecules. Concurrently, this configuration significantly reduces the energy barrier of the *OOH intermediate. These synergistic effects collectively optimize the electrocatalytic performance for H₂O₂ production under alkaline conditions. As expected, the Fe(CN)₆-ZnO-V_O delivers a significantly increased current density of 130 mA cm⁻² that is much higher than ZnO (32 mA cm⁻²), as well as a superior H₂O₂ production rate of 9.41 mol g_cat⁻¹ h⁻¹ and a high faradaic efficiency of exceeds 90%. Our study highlights the crucial role of interfacial hydrogen-bonding connectivity and provides theoretical and technical guidance for developing reliable strategies to enhance the electrocatalytic properties of 2e⁻ORR.

Due to their versatile and tunable surface and bulk chemistry, MXenes have great potential as electrocatalysts for batteries and supercapacitors. When compared with other electrocatalytic processes, in electrocatalytic reactions, MXenes could improve ion diffusion and charge transfer by either providing functional groups binding to the surface metals to block the diffusion path or offering additional adsorption sites for metal cations or intermediate products on the material surface, so the electrocatalytic activity of MXenes should be sensitive to the surface configuration. Very recently, researchers revealed that introducing defects and strictly tuning the electronic property of the MXene surface could greatly improve its electrocatalytic efficiency; however, the exact mechanism by which defects could improve the electrocatalytic properties of MXenes was still unclear. In this study, authors classify surface defects in MXene, discuss the formation mechanism of each kind of defect, and demonstrate the application of atomic-level characterization tools to track the evolution of defects. Furthermore, based on the defect mechanics principles, we propose a rational design approach for MXene surface structures. Additionally, this paper discusses the development and application of defect structures in electrocatalytic efficiency improvement. Based on the analysis of the challenges existing in the MXene electrocatalysis, a future research direction is proposed. In this review, we establish a conceptual framework for MXene applications in electrocatalysis. This study advances the development of MXene materials in energy systems, provides the defect design strategies for researchers in further investigation on MXenes, and offers the emerging trends in this field.

Coupling lithium metal with gel polymer electrolytes (GPEs) has been demonstrated as an effective strategy to enable stable lithium metal batteries (LMBs). However, the current design of GPEs faces difficulties in simultaneously achieving satisfactory mechanical properties and efficient and selective ion transport. Here, we present the fabrication of ultrastrong and hierarchically nanoporous cellulose gel electrolytes via poly(ionic liquid)-induced interfacial coacervation of cellulose nanofibrils. The nanofibrils GPE with a cascade ion-conduction network spanning from molecular-scale channels to mesopores enables dual-mode Li⁺ transport through nanoconfinement and interstitial ion hopping. This mechanism effectively blocks anion movement while achieving selective Li⁺ transport with a high transference number of 0.7 and a high ionic conductivity of 0.65 mS cm⁻¹. The GPE enables stable cycling of high mass loading (LiFePO₄, 16 mg cm⁻²) LMBs and high-temperature (80°C) LMBs. Specifically, the LMB with a high LiFePO₄ loading of 12 mg cm⁻² delivers stable cycling life over 600 cycles, maintaining 87% capacity retention. Furthermore, the assembled 635 mAh pouch full cell demonstrates excellent stability with a high capacity retention of 91.7% after 1500 cycles. This study offers a novel strategy for the development of robust and ion-selective GPEs for stable LMBs.

The electrocatalytic CO₂ reduction reaction (CO₂RR) offers a viable solution for the conversion and storage of renewable energy. Utilizing electronic metal-support interactions (EMSI) to adjust the electronic properties of metal catalysts has demonstrated effectiveness in enabling highly selective CO₂ electroreduction. Here, a cleverly designed ternary composite is presented, which is synthesized by using nitrogen-doped hollow carbon spheres (NHCS) as the substrate and coating them with poly(3,4-ethylenedioxythiophene) (PEDOT) to form a PEDOT/NHCS support for anchoring Au nanoparticles. This innovative design enables the catalyst to reach a stunning 98.21% at −0.8 V versus RHE, achieving an extraordinarily high Faradaic efficiency for CO (FE_CO) over a broad potential window (−0.6 to −1.5 V vs. RHE). The result is mainly due to the Au–S bond between the S in the PEDOT thiophene ring and the metal Au, which induces electron transfer, causing the d-band center of the Au atoms to shift negatively. The hydrophobic surface of PEDOT and the hollow structure of NHCS synergistically construct an interface of “CO₂-philic and H₂O-phobic.” This interface, in coordination with the Au NPs, enhances CO₂ adsorption, stabilizes the *COOH intermediate, accelerates the desorption of *CO, and simultaneously weakens the competitive adsorption of *H, effectively suppressing the HER.

Electrocatalytic nitrate reduction represents a sustainable strategy to mitigate nitrogen cycle imbalance by converting NO₃⁻ into NH₃ under ambient conditions. However, conventional catalysts usually suffer from limitations in activity–selectivity–stability synergy. Herein, we propose a rational design guided by density functional theory calculation to engineer defect-coordinated iron single-atom catalysts (Fe─N₂, Fe─N₃, and Fe─N₄) for efficient electrocatalytic nitrate reduction. The superior Fe─N₂ catalyst with asymmetric coordination geometry achieves an unprecedented nitrate-to-ammonia conversion efficiency of 29,700 mg N/g at −0.65 V (vs. reversible hydrogen electrode) with 100% NH₃ selectivity as well as exceptional durability, maintaining > 95% activity over 480 h of continuous operation. In situ X-ray absorption near-edge structure directly captures dynamic valence-state modulation of Fe sites under reaction conditions, coupled with stable Fe–N coordination, confirming electron-density enrichment at active sites and robust structural integrity. Online differential electrochemical mass spectrometry and in situ Raman spectroscopy reveal the sequential reduction pathway (NO₃⁻ → NO₂⁻ → NO → NH₂OH → NH₃), directly correlating the asymmetric Fe─N₂ coordination with optimized reaction kinetics. Practical validation in a continuous-flow reactor demonstrates > 98% nitrogen removal efficiency for 1.0 L nitrate-contaminated wastewater (100 ppm NO₃⁻–N) within four cycles through using this Fe─N₂-based electrode, achieving World Health Organization (WHO)-compliant drinking water standards. This work establishes asymmetric Fe─N₂ coordination as a paradigm for high-performance nitrate reduction, bridging computational design with scalable synthesis to advance sustainable nitrogen valorization and environmental remediation.

Developing efficient and durable Pt–C catalytic cathodes is crucial for enhancing Li–O₂ batteries; however, it remains a significant challenge. Here, we designed a self-supporting three-dimensional Pt–C₆₀@GO cathode and demonstrated its flexible use in the large-area battery assembly. Pt–C₆₀@GO cathode features parallel structurally continuous graphene oxide films, within which fullerene nanospheres are uniformly embedded, and platinum nanodots that are also equably attached, forming a longitudinally ordered stacking structure. The obtained cathode exhibits highly exposed platinum active sites with robust Pt–C and Pt–O bonding interactions, demonstrating remarkable electrocatalytic activity and electrochemical stability. This enables promising electrochemical performance, including a high areal capacity of 3.70 mAh cm⁻², a low cell overpotential of 0.48 V, and an excellent cycle stability exceeding 100 cycles. Notably, this self-supporting electrode design facilitates the flexible battery assembly, where a single-layered Pt–C₆₀@GO//LiMg pouch-cell displays a high energy density of 324.6 Wh kg⁻¹ and a stable cycle life over 10 cycles in air.

Dry electrodes with polytetrafluoroethylene (PTFE) binders are promising candidates for sustainable lithium-ion batteries owing to their low cost, environmental sustainability, and compatibility with high-mass–loading designs; however, the application of PTFE in anodes is hindered by its irreversible reduction at low potentials and degradation mechanisms, which remain under investigation. This study elucidates the influence of the molecular weight of PTFE on the electro-chemo-mechanical stability of dry-processed graphite anodes. Dry electrodes with a low content (0.5 wt.%) of high-molecular-weight PTFE show ultra-high areal capacities of ~11, 22, and 33 mAh cm⁻². Under lean electrolyte conditions, pouch cells incorporating the optimized high-molecular-weight PTFE electrode attain a high volumetric energy density (> 840 Wh L⁻¹ at 0.1 C) and a capacity retention of 76% over 300 cycles—significantly outperforming conventional wet-processed electrodes (> 790 Wh L⁻¹ at 0.1 C, capacity retention ≈56%). This study provides fundamental insights into the degradation of PTFE and presents a viable pathway toward scalable, high energy density, and environmentally sustainable battery manufacturing.

Photocatalytic CO₂ reduction involves multiple proton-coupled and multi-electron transfers, leading to a plethora of reaction pathways and consequently unpredictable products. The unique electronic structure and unsaturated coordination environment of single-atom photocatalysts can influence the reaction pathways of CO₂ photoreduction, enhancing the yield of a target product. Herein, we rationally design the In single-atom photocatalyst (In-NTO) containing isolated In^δ+–N₃O₂ atomic interface sites for highly efficient and selective CO₂-to-CO photoreduction. This distinctive atomic configuration not only reduces the overall activation energy barrier but also transforms the key *CO desorption step from an endoergic to an exoergic one, thereby altering the reaction pathway to selectively produce CO rather than CH₄. Consequently, the 0.25 wt% In-NTO exhibits high selectivity (95.9%) for photocatalytic CO₂-to-CO conversion, with a rate of 6.34 µmol g⁻¹ h⁻¹. This work offers a novel strategy for modulating the reactivity and product selectivity of photocatalytic CO₂ reduction toward desired products by constructing single-atom sites with heteroatomic coordination.

The electrocatalytic reduction of CO₂ (CO₂RR) to methane (CH₄) using renewable electricity represents a pivotal technology for closing the anthropogenic carbon cycle. However, achieving high CH₄ Faradaic efficiency at industrially relevant current density remains challenging. This is primarily due to the complex multiple adsorption, activation, and reaction steps for CH₄ production, in which each process needs to occur efficiently at its matching catalytic active sites, so the kinetic bottlenecks exceed the capacity of single or dual-site catalysts. To address this, we engineered a Cu/Al-based multi-site heterogeneous electrocatalyst featuring atomically dispersed Cu clusters (1.5 wt.%) on a γ-Al₂O₃ matrix. Experimental and theoretical studies reveal that Cu and γ-Al₂O₃ sites predominantly serve as CO₂ (forming *CO) and H₂O molecule (yielding *H) activation centers, respectively, whereas Cu/γ-Al₂O₃ interfacial sites primarily accelerate the *CO and *H coupling to form rate-determining step intermediates (*CHO). The optimized Cu_1.5 wt.%/γ-Al₂O₃ multi-site catalyst exhibited a high CH₄ Faradaic efficiency of 72% at the current density of 500 mA cm⁻², outperforming the reported Cu-based single-site and dual-site catalysts. This study establishes combinatorial site engineering as a paradigm for overcoming scaling relations in multi-step CO₂ hydrogenation, with broad applicability in catalyst design.

Halide solid-state electrolytes (HSSEs) have gained significant attention as key components for all-solid-state lithium ion batteries due to their notable advantages, including high ionic conductivity (> 1 mS cm⁻¹), wide electrochemical window (> 4 V vs. Li/Li⁺), and good compatibility with high-voltage cathodes. Despite progress, major challenges such as ionic conductivity, air stability, and interface compatibility still remain. This review systematically summarizes their representative classifications (e.g., Li_a-M-X₈, Li_a-M-X₆, Li_a-M-X₄, Li_aM_bO_cX_d, M = In, Y, Al…; X = Cl, F, Br…), synthesis methods (e.g., solid phase, liquid phase, gas phase), and ion conduction mechanisms (e.g., vacancy-driven transport). The merits and demerits of different synthesis methods are analyzed, and the factors affecting ion conductivity are also discussed. Moreover, various modification strategies (e.g., structure optimization, doping, and surface coating) are analyzed to address the above issues. Meanwhile, research guidelines for developing advanced HSSEs are also proposed. Additionally, we provide a systematic outlook on HSSEs in terms of novel synthesis methods and interface modification technologies (such as plasma and supercritical fluid technologies), high-precision characterization methods for interface components (such as solid-state nuclear magnetic resonance), artificial intelligence (AI)-assisted mechanism analysis, and material synthesis. This review offers new research insights into the design and development of advanced solid-state electrolytes for energy storage.

Phase-pure two-dimensional (2D) interfacial passivation has emerged as an effective strategy for addressing the intrinsic instability and interfacial defects of three-dimensional (3D) perovskite absorbers. However, conventionally formed 2D layers often suffer from mixed-n phases, heterogeneous quantum-well distributions, and disordered orientation, which impede charge transport, distort energy-level alignment, and accelerate structural degradation. In this review, we elucidate the thermodynamic and kinetic origins of mixed-phase formation and discuss how dimensional heterogeneity adversely impacts carrier dynamics and device stability. We then summarize recent advances in achieving phase-pure 2D perovskite interlayers that enable precise n-value control, favorable crystal orientation, and optimized interfacial energetics. These strategies yield highly ordered 2D/3D heterostructures that effectively suppress ion migration, mitigate non-radiative recombination, and significantly enhance long-term operational stability. Finally, we outline the remaining challenges and emerging opportunities for scalable, phase-pure engineering toward high-efficiency and stable perovskite photovoltaic technologies. Overall, this review provides a unified framework linking phase purity, interfacial ordering, and device stability, offering guidance for the development of next-generation robust perovskite photovoltaics.

Although solar-driven interfacial evaporation offers a sustainable pathway for desalination and wastewater remediation, its practical implementation remains limited by both the high vaporization enthalpy and rigid hydrogen-bond network of water and performance degradation in complex water matrices. This study introduces a dual-regulation strategy that integrates internal structural optimization with external-field physical modulation. In particular, an Fe-catalyzed pyrrole polymerization process yields a carbon-based aerogel (CPP) with integrated ferromagnetism and enriched pyrrolic nitrogen sites. This synergy increases the intermediate-water fraction, reduces vaporization enthalpy, and accelerates phase-transition kinetics. Under one-sun illumination (1 kW m⁻²), the CPP evaporator achieves an evaporation rate and efficiency of 2.78 kg m⁻² h⁻¹ and 84.0%, respectively, without magnetic assistance. After applying a 10 mT magnetic field, these values increase to 3.30 kg m⁻² h⁻¹ and 99.7%, respectively. Moreover, the system demonstrates stable salt self-cleaning in seawater, resilience in organic wastewater, and multifunctionality in pollutant removal, achieving a tetracycline degradation rate of 89% when coupled with a solar-driven advanced oxidation process. This study offers a generalizable framework that couples structural design with external-field modulation for next-generation solar evaporation systems.