Photocatalytic CO2 reduction represents a promising strategy to address global energy and environmental challenges, and the development of high-performance catalysts is a critical process. However, due to the limitations of the number of accessible active sites and the efficiency of charge separation, the activity of most catalysts is unsatisfactory. Herein, we proposed a dual-functional strategy that utilized short-range interactions to immobilize metal porphyrins (MPor) with single active sites within the pores of PCN-222, thereby obtaining novel catalysts (MPor@PCN-222). CoPor@PCN-222 exhibits the best catalytic activities, with a CO production rate of 6790.3 mu mol g- 1 h- 1. The total production rate of CoPor@PCN-222 is 42 times that of the CoPor catalyst, and it surpasses most reported MOF-based and molecular catalysts. Experiments and theoretical results have confirmed that the short-range interactions between CoPor and PCN-222 provide convenient channels for electron transfer, thereby significantly enhancing charge separation efficiency. In addition, the synergistic effect between the guest CoPor and the host PCN-222 framework also makes a significant contribution to the enhancement of catalytic activity. On the one hand, PCN-222 promotes the adsorption and enrichment of CO2 around the active sites during the reaction process, facilitating the mass transfer process of the reaction. On the other hand, atomically dispersed Co sites effectively activate CO2 and substantially lower the energy barrier for the formation of the critical *COOH intermediate. This study clarifies the crucial role of interactions within the composite system on performance and provides a feasible example for the construction of highly active and stable CO2 photoreduction catalysts.

The exploration of solid-state lithium–air batteries operating in humid air is hindered by severe alkaline corrosion from LiOH discharge products. This preview highlights a hierarchical high-throughput screening approach to address this challenge by combining machine learning potentials with density functional theory calculations. Evaluating over 320,000 compositions, 209 alkaline-stable candidates are identified, and critical trade-offs between ionic/electronic conductivity and alkaline resistance are revealed, providing a rational roadmap for durable material design.

In geometrically frustrated lattices, flat bands can arise from destructive quantum interference, providing an ideal platform for exploring strong electron correlations. However, direct real-space evidence of their predicted atomic-scale electron localization remains elusive. By employing scanning tunneling microscopy/spectroscopy, with a focus on quasiparticle interference imaging, we demonstrate unambiguous atomic-scale localization of flat band electrons in the kagome metal Fe 3 Sn 2 . Crucially, quasiparticle interference imaging reveals a complete suppression of scattering wavevectors and standing waves exclusively at the flat band energy, indicating the absence of long-range coherent propagation. This disappearance of the quasiparticle interference signal, attributable to the non-propagating wavefunctions inherent to the kagome flat band, directly confirms real-space electron localization. These findings resolve the microscopic link between quantum interference and localization of flat band electrons, paving the way for engineering correlated quantum states.

Polymer electrolytes (PEs) are widely regarded as a promising platform for solid-state batteries (SSBs), offering the potential to simultaneously achieve high energy density with improved safety. However, in current literature, PEs spanning liquid-percolated gels, liquid-assisted quasi-solids, and truly polymer-governed solids are often indiscriminately grouped as solid polymer electrolytes (SPEs), obscuring their distinct ion transport mechanisms, interfacial behaviors, and practical performance constraints, and leading to misleading performance comparisons and unrealistic expectations regarding solid-state operation. Herein, we establish a mechanistic framework that categorizes PEs into gel polymer electrolytes (GPEs), quasi-solid polymer electrolytes (QSPEs), and all-solid polymer electrolytes (ASPEs) based on their dominant ion-solvation environment and transport pathways. By systematically analyzing the ion-transport mechanisms, interfacial behaviors, and performance-limiting features associated with each PE class, we clarify their defining characteristics and mechanism-imposed limitations. Accordingly, we outline category-specific research priorities and highlight the necessity of mechanism-driven materials design, transparent definitions and reporting, and application-relevant benchmarking. This unified Perspective lays a foundation for consistent interpretation, meaningful comparison across PE systems, and more rational materials design toward the advancement of PE-enabled SSBs.

Exploring the interaction between perovskite metal oxides and iodide ions greatly contributes to understanding the influence of iodide ions on their physicochemical properties and leading to higher performance. Here, we investigate for the first time the interaction between iodide ions and uniformly distributed Ag based perovskite metal oxides (AgBO3) including AgBiO3, AgVO3 and AgNbO3. We find that iodide ions can induce the etching of AgBiO3 at room temperature, resulting in a significant change in the crystal structure and morphology. Iodide ions can selectively extract silver atoms from AgBiO3, forming AgI crystals and Bi2O3 skeletons with a well-developed porosity and high surface area. In comparison, the etching products of AgVO3 are AgI and VO3- ions, with VO3- ions being soluble in water. Furthermore, experimental characterization results from XRD and SEM, along with DFT calculations, indicate that iodine ions cannot spontaneously etch AgNbO3. Therefore, the etching results of iodine ions on Ag based perovskite metal oxides are closely related to their crystal structure, as well as the properties and electronic characteristics of the B site metal elements. Based on the unique etching reaction of AgBiO3, AgBiO3 has been innovatively applied as an effective adsorbent for radioactive I- in contaminated water or nuclear effluents. Moreover, the gentle etching process is a powerful synthetic method for generating porous Bi2O3. The Bi2O3 nanostructure with unique porosity is found to be an excellent catalyst for the reduction of 4-NP (4-nitrophenol).

The inherent flammability of poly (lactic acid) (PLA) severely restricts its range of applications, whereas circular economy principles require full component recovery of waste PLA components. Conventional flame-retardant modifications often induce excessive PLA degradation during melt processing and contaminate monomer streams in chemical recycling, creating a long-standing conflict between fire safety and recyclability. In this work, a phosphorus/nitrogen-containing flame retardant, designated CEDCE, was synthesized. With only 3.0 wt% CEDCE loading, the PLA/CEDCE composite attained a limiting oxygen index of 28.2% and achieved a UL-94 V-0 rating, accompanied by suppressed melt dripping and markedly reduced heat release rate and total heat release, all while preserving favorable mechanical properties and processability. During chemical recycling, the zwitterionic nature of CEDCE not only enables its own efficient recovery through pH adjustment but also becomes activated under methanolysis conditions to catalyze PLA depolymerization, thereby allowing simultaneous recovery of high-purity methyl lactate and reusable flame retardant without any external catalyst. This study provides an innovative strategy to simultaneously improve the functionality, comprehensive performance, and chemical recyclability of PLA-based materials for sustainable circular development.

The relaxor ferroelectric polymer poly(vinylidene fluoride-co-trifluoroethylene-co-chlorofluoroethylene) (P (VDF-TrFE-CFE), PVTC), with a high dielectric constant and unique segmental structure, effectively promotes lithium salt dissociation and optimizes ion transport, serving as an optimal matrix for high-performance solidstate electrolytes. However, single-component PVTC electrolytes face key challenges including insufficient mechanical strength, limited lithium dendrite suppression capability, and poor interfacial stability. Herein, a dualfiller synergistically enhanced composite solid electrolyte (CSE) is fabricated by simultaneously incorporating mesoporous Santa Barbara Amorphous-15 (SBA-15) and zirconium dioxide (ZrO2) nanoparticles into the PVTC matrix. The ordered mesoporous structure of SBA-15 provides fast lithium-ion transport pathways; ZrO2 nanoparticles promote lithium salt dissociation via Lewis acidic zirconium sites, and its rigid skeleton suppresses the growth of lithium dendrites. The as-fabricated CSE delivers an ionic conductivity up to 3.91 & times; 10- 4 S cm- 1 at room temperature. Full cells with lithium iron phosphate (LiFePO4, LFP) cathode exhibit a capacity retention of 82% after 100 cycles at 0.05C, and maintain approximately 47% of their initial discharge capacity even after an extended cycling for 1200 cycles. Li symmetric cells show stable cycling for 2175 h at 0.05 mA cm-2 with outstanding interfacial stability. This dual-functional synergistic strategy offers a facile and effective route for developing next-generation high-safety solid-state lithium batteries.

Chloramphenicol (CAP) has evolved from a widely used antibiotic to a persistent pollutant that is difficult to manage. We employed photocatalysis to address the pollution that it caused. Given the similarity in requirements for active layer materials between photocatalysis and solar cells, we selected outstanding materials already employed in bulk heterojunction organic solar cells (BHJ-OSCs) to construct the catalyst. We selected PTQ10, which is low-cost and readily synthesized, as the donor and ITIC-Th and IEICO-4F, which can broaden the absorption range, as the acceptors, thereby constituting two distinct D-A heterojunction active layers. We immobilized them onto coconut shell charcoal (CSC) obtained from agricultural byproduct recycling, yielding two catalysts: PTQ10:ITIC-Th/CSC and PTQ10:IEICO-4F/CSC. They were able to degrade 97% of high-concentration CAP within 15 min under visible light irradiation and remained stable for over 20 cycles. We further investigated the influence of molecular structure on photocatalytic processes as follows: 1) ITIC-Th exhibits a larger dipole moment and more favorable band structure, resulting in enhanced charge separation efficiency; 2) ITIC-Th possesses reduced steric hindrance, exposing more active reaction sites; and 3) ITIC-Th demonstrates a broader light absorption range with more complete absorption of visible light. The above three points enable PTQ10:ITIC-Th/CSC to generate more •O2- and degrade CAP more efficiently. This work is expected to provide some ideas and help with environmental pollution control and photocatalyst design.

ABSTRACT Hard carbon (HC) anode in sodium‐ion batteries suffer from low initial Coulombic efficiency and irreversible capacity loss, limiting practical energy density and cycle life of SIBs. While direct‐contact presodiation of HC has been proposed to increase the initial Coulombic efficiency of SIBs, but its low utilization efficiency can cause residual Na on the HC surface, resulting in rapid degradation and even safety concerns. Herein, we proposed a soft‐contact presodiation (SCP) method, which can remove and recycle Na source and therefore greatly improve the utilization of the Na source and safety of SIBs. The SCP‐treated HC anode achieves a ≈30.0% increase in ICE when paired with a NaNi 1/3 Fe 1/3 Mn 1/3 O 2 cathode, while maintaining minimal temperature rise (Δ T ≈1.3°C) during treatment. The resulting SCP‐HC exhibits exceptional thermal stability with negligible exothermic activity at 125.0°C and remains chemically stable for over 3.0 days. Through multimodal analysis, we reveal an adsorption‐dominated compensation mechanism where replenished Na participates in solid electrolyte interphase formation while simultaneously occupying adsorption sites as metallic clusters. The pouch cell incorporating SCP‐HC anode delivers 90.6% ICE and retains 80.0% capacity after 150 cycles. This work establishes a safe, efficient, and economically viable presodiation platform that paves the way for practical high‐energy sodium‐ion batteries.

Developing next-generation batteries that are high-energy, low-cost and eco-friendly is crucial for industrial applications. Lithium-rich manganese-based oxide positive electrodes offer substantial specific energy, enabled by their high specific capacity at high charging potential (>4.6 V versus Li/Li+). However, stable operation at such high potentials remains challenging, as most electrolytes rely on environmentally unfriendly fluorinated solvents. Here we identified α-oxidation of the carbonyl group as the main oxidation mechanism of carboxylate esters. By removing all the reactive α-hydrogens of methyl acetate, we demonstrate that methyl trimethylacetate is a non-fluorinated, high-potential-stable solvent. This solvent exhibits outstanding oxidative stability up to 5.6 V versus Li/Li+, and electrochemical cells using methyl-trimethylacetate-based electrolytes maintain stable cycling at 4.6/4.7 V, outperforming many fluorinated systems. An industrial-scale 7.2-Ah pouch cell reached a maximum specific energy of 652.4 Wh kg-1 with 94.5% capacity retention after 28 cycles at 0.1 C/0.2 C. This work provides a simple molecular design strategy that addresses specific energy, cost and sustainability in next-generation high-voltage lithium batteries.

Irreversible dissolution of redox-active transition metals during the oxygen evolution reaction remains a major challenge in developing durable water electrolysis catalysts, particularly for Fe-containing spinel oxides. Despite strategies to mitigate Fe dissolution, its atomistic pathway and mechanism remain unclear. Here, we combine static and dynamic ab initio modeling with electrochemical tests to investigate Fe dissolution in NiFe2O4 and CoFe2O4 spinels. Instead of viewing Fe instability as an intrinsic property, we show that it arises from bond strength competition within the M-O-Fe (M = Ni or Co) linkages. A stronger M-O bond (as in Co-O) weakens the adjacent Fe-O bond under electrochemical bias, making Fe dissolution more favorable in CoFe2O4 than that in NiFe2O4. Such asymmetric bond competition leads to enhanced Fe dissolution while simultaneously facilitating surface reconstruction and catalyst deterioration. This work establishes bond competition as a decisive descriptor for metal dissolution, offering practical guidelines for designing stable OER catalysts.

Bi2S3 has been considered as an extremely attractive anode for potassium energy storage due to its low cost, good safety, easy synthesis and high theoretical capacity. Nevertheless, it possesses a poor potassium storage performance in practical application because of its sluggish kinetics and severe volume change. To address these challenges, the designed nitrogen-doped carbon-modified Bi2S3 (Bi2S3@NC) nanofibers have been successfully prepared by an electrospinning route and carbonization process. In this designed nanocomposite, the nanosized Bi2S3 particles are uniformly distributed within the one-dimensional mesoporous nanofibers. The constructed mesopores can greatly buffer the volume change of Bi2S3 nanocrystals during the K+ insertion and extraction. Meanwhile, the one-dimensional conductive networks formed by nitrogen-doped carbon fibers are helpful to promote the electronic conductivity of Bi2S3 nanoparticles. This obtained Bi2S3@NC anode exhibits excellent rate capability (467 mAh/g at 1 A/g) and good cyclic performance (79% capacity retention ratio at 5 A/g for 1000 cycles). This study offers a good approach for constructing advanced electrode materials with fast electrochemical reactions.

By controlling the morphology of CeO2 and dispersing bimetallic CuxFey on its surface, different morphological CuxFey/CeO2 composites were constructed. XRD, SEM, TEM, N2O pulse titration, N2 adsorption/desorption, and XPS characterizations show that rod-shaped CeO2 (CeO2-R) with a higher surface area enables the highly dispersing of Cu and Fe species, provides abundant oxygen vacancies, enhances the CO2 adsorption and dissociation capabilities. Competitive adsorption of H2/CO2, H2-TPR, CO2-TPD, DFT calculations of adsorption capacity, and in situ DRIFTS reveal that modulating the atomic ratio of Cu/Fe on CeO2-R accelerates the H2 dissociation, suppresses the excessive formation of CHx* intermediates to methane, and produces HCOO* and CO*. Metal-support interaction strengthens the CO2 adsorption and C-C bond coupling, thereby improving the CO2 hydrogenation to ethanol. Thus, Cu1Fe2/CeO2-R was found to be highly efficient, with a CO2 conversion of 31.7% and an ethanol selectivity of 23.6% under T = 320 °C, P = 2.0 MPa, H2/CO2 = 3 (volume ratio), and GHSV = 12,000 mL/(gcat·h).

The lithium bond is an essential weak interaction in lithium batteries, critically influencing ion transport, interfacial reactions, and electrochemical performance. Herein, the current understanding of lithium bond chemistry is systematically discussed across different lithium species and their associated electrochemical behaviors. We first discuss the lithium bonds formed between monomeric lithium ions and guest molecules, with an emphasis on their structural characteristics and functional roles in both liquid and solid phases. The discussion is then extended to lithium complexes, focusing on how the lithium bond drives short-range and long-range structure organization and corresponding functionality. Furthermore, the synergy between the lithium bond and strong ionic/covalent bonds is highlighted, emphasizing how their balance can inform the rational design of advanced lithium batteries. Finally, future research directions in lithium bond chemistry are outlined, aiming to accelerate the development of advanced lithium batteries and enrich the chemical understanding of weak interactions in the broader context of modern chemistry.

Halide materials have emerged as a promising solid electrolyte candidate for all-solid-state batteries owing to their high ionic conductivity and tunable electrochemical stability. Beyond this established role, they also offer an underexplored opportunity to contribute to energy storage as potential capacity contributors through their intrinsic redox chemistry. Herein, we synthesize the nascent field of halide redox chemistry, spanning both metal cations and halogen anions, and identify a core design principle that involves strategically matching the reversible redox voltage window of halides to the operating voltage of high-capacity electrodes. Beyond cation-centric redox, we elucidate the distinct reversibility of halogen anions (Cl, Br, and I) and illustrate their role in enhancing battery performance. By extending the function of halides from ion transport to coupled redox participation, this perspective outlines new directions for the design of next-generation all-solid-state batteries.

Electrochemical lithium (Li)-mediated nitrogen (N2) reduction could enable production of ammonia (NH3) at ambient temperatures and pressures, offering a route to reduce carbon emissions in the chemical sector. However, NH3 productivity is often limited by sluggish Li-ion desolvation and diffusion at the solid electrolyte interphase (SEI). Here, we present a concerted desolvation:diffusion layered SEI architecture that provides abundant Li-ion flux for efficient N2 conversion toward NH3 production at high current densities. The SEI comprises stacked inorganic layers with low ion-binding affinity and high ion-conductivity functionalities that increase Li-ion flux by two orders of magnitude. This design strategy achieved N2 electroreduction in a 2 M lithium difluoro(oxalato)borate electrolyte with a Faradaic efficiency of 98% and an energy efficiency of 21% for NH3 production at 100 milliamperes per square centimeter (mA cm-2). The system sustained an 80% Faradaic efficiency over 40 hours, after which performance declined.

Lithium-sulfur (Li-S) batteries are promising in realizing high energy density. Employing weakly solvating electrolytes (WSEs) further improves the anode stability. However, the lithium polysulfide (LiPS) redox kinetics is hindered in WSEs, and the underlying mechanism remains unclear. Herein, the LiPS kinetics in WSEs is quantitatively deciphered using rotating disk electrode analysis. The electron transfer number during oxidation is reduced in WSEs, evidencing intrinsically suppressed oxidation extent. Meanwhile, the diffusion coefficient and the electrolyte viscosity concurrently increase, implying a reduced LiPS hydrodynamic radius in WSEs based on the Stokes-Einstein relation and corresponding to inhibited LiPS molecular aggregation. Attributed to the reduced aggregation, WSE-based Li-S batteries exhibit record-low-temperature performances, delivering 8.0 mAh cm-2 and 303 Wh kg-1 at 0 degrees C in 6 Ah-level pouch cells. This work establishes a new kinetic analysis methodology to guide rational electrolyte design and highlights the promise of WSEs to enable low-temperature Li-S batteries.

Dehydroxylation of kaolinite is a pivotal step in the preparation of supplementary cementitious materials and geopolymer precursors, yet its atomistic mechanism remains elusive. By integrating static DFT calculations (CI-NEB/DIMER), metadynamics simulations, and wave function analyses (MBIS charges, FBO, sobEDA), a dehydroxylation mechanism dominated by proton (H+) migration was revealed. Kinetic simulations at 1200 K identified interlayer migration (Path I, Delta G double dagger= 216.64 kJ & sdot;mol-1) and adjacent surface migration (Path II, Delta G double dagger= 141.52 kJ & sdot;mol-1) as feasible pathways. Energy decomposition analysis indicated that Path I was governed by Pauli repulsion, whereas Path II was controlled by the cost of bond breaking. The calculated barriers for both paths fell within the experimental activation energy range (140-255 kJ & sdot;mol-1). Thermogravimetric simulations quantitatively mapped the temperature domain contributions of Path I and Path II, thereby validating, for the first time at the macroscopic scale, their competing mechanism. The "static-dynamic-electronic-macroscopic" multiscale framework established herein offered a universal theoretical model for understanding the dehydroxylation of hydroxyl bearing solids.