The practical applications of lithium-sulfur (Li─S) batteries are impeded by sluggish conversion kinetics of lithium polysulfides (LiPSs) and uncontrolled Li dendrite growth. While introducing single-atom catalysts (SACs) stands out as a promising strategy to overcome these issues, the p-block SACs exhibit great potential. However, the relationship between their synergistic regulation and atomic structure remains unclear. Here, by leveraging the p-electron delocalization induced by the p-π conjugated effect, p-block Se SACs were proposed to synergistically regulate the lithium/sulfur electrochemistry. The experimental and theoretical results demonstrate that the unique Se-C2 coordination structure of Se SACs leads to activated p-electrons, which not only facilitates LiPSs conversion by p-p hybridization but also generates a uniform current distribution to guide Li plating and stripping behavior. Consequently, the Li─S batteries assembled with Se SACs demonstrate a low capacity decay rate of 0.056% per cycle over 1000 cycles at 1 C and achieve a high areal capacity of 5.58 mAh cm-2 under a high sulfur loading of 6.41 mg cm-2 and a low electrolyte/sulfur ratio of 8.3 µL mg-1. This work elucidates the synergistic regulation of Se SACs from atomic orbital level and enlightens the application of p-block SACs in Li─S batteries.

The compositional heterogeneity of post-consumer plastic waste, exemplified by prevalent polyethylene (PE)/polypropylene (PP) mixtures (>50% of the plastic market), severely complicates recycling. Kinetic disparities between PE and PP during chemical recycling create significant conversion gradients, limiting valued product yield and process viability. Here, leveraging strong interfacial coupling between ruthenium oxides and rutile TiO2, we construct highly active, epitaxial RuOx sites enabling efficient one-pot co-conversion of PE/PP mixtures with a high liquid yield of 95.02%, while maintaining a low 0.62% gas yield. Compared to conventional Ru nanoparticles, the epitaxial RuOx structure provides additional dehydrogenation sites for PP activation, which promotes carbon-metal back-donation to weaken C-C bonds, thus exhibiting comparable activation capabilities toward both 3C-2C bond in PP and 2C-2C bond in PE. This unique epitaxial catalyst enables highly efficient co-hydrogenolysis of mixed polyolefins, establishing a practical approach for their upcycling.

Lithium-sulfur (Li-S) batteries hold great promise for high-energy-density energy storage applications but are plagued by the severe shuttle effect and sluggish conversion kinetics of lithium polysulfides (LiPSs). We herein report a d-p-f orbital coupling strategy to tackle these critical challenges by incorporating Eu 4f orbitals to activate both metallic (Ni) and non-metallic (Se) sites of NiSe. The imported Eu atoms could induce essential Ni 3d and Se 4p orbital reconstruction through gradient d-p-f coupling, thereby optimizing the band center alignment between NiSe and LiPSs. Such electronic reconstruction strengthens both d-p hybridization between Ni and LiPSs and s-p hybridization between Se and LiPSs, which can not only enhance the chemisorption affinity toward LiPSs but also accelerate interfacial charge transfer kinetics, leading to suppressed shuttle effect and boosted LiPSs conversion kinetics. Therefore, the Li-S batteries assembled with Eu incorporated NiSe deliver exceptional electrochemical performance with a high specific capacity of 896.2 mAh g-1 at 4 C and a retained areal capacity of 5.66 mAh cm-2 under a high sulfur loading of 5.94 mg cm-2 after 100 cycles. This work underscores the critical role of rare-earth 4f orbital coupling for modulating the active sites to construct high-efficiency electrocatalysts for Li-S batteries and beyond. (c) 2025 Science Press and Dalian Institute of Chemical Physics, Chinese Academy of Sciences. Published by Elsevier B.V. and Science Press. All rights are reserved, including those for text and data mining, AI training, and similar technologies.

The direct regeneration of spent lithium-ion batteries has attracted considerable attention due to its potential to maximize economic benefits while minimizing environmental impacts. However, fluorine-containing contaminants severely interfere with the regeneration process through chemical interactions, often resulting in the cathode fluorination. Moreover, constrained by the technical limitations inherent in the original synthesis processes of waste electrodes, the cycling stability of regenerated cathode materials struggles to meet the current technical standards. Herein, we elucidate the underlying mechanisms of F-induced degradation in spent cathode materials and develop a flash Joule heating (FJH) technique with a Ca(OH)2 medium to achieve the coupling effect of fluorination inhibition and lattice stabilization in a single processing step. The addition of Ca(OH)2 can effectively capture the secondary HF, mitigating its corrosion of the cathodes to form a metal fluoride. Furthermore, the high temperature during FJH treatment facilitates in situ Ca doping into the LiCoO2 lattice, enhancing its electronic and ionic conductivity. Following hydrothermal relithiation and a brief sintering regeneration process, the regenerated Ca-doped LiCoO2 demonstrates a high capacity of 150.2 mAh/g (0.1 C) and enhanced cycling stability from 64.3 to 91.2% compared to that without Ca doping. This work provides a mechanistically guided and industrially adaptable strategy for the efficient regeneration of fluorinated cathodes, advancing the practical implementation of sustainable battery recycling.

Aqueous zinc-iodine batteries (ZIBs) based on four-electron I-/I0/I+ redox chemistry hold great promise for high-energy-density energy storage. However, their practical deployment faces critical challenges, mainly including the polyiodide shuttle effect, hydrolysis of I+, sluggish iodine conversion kinetics and poor reversibility of Zn anodes. Herein, we propose a low-concentration electrolyte strategy by employing choline chloride (ChCl) as a dual-functional additive to achieve highly efficient four-electron ZIBs. It is demonstrated that Ch+ not only suppresses polyiodide shuttle by strong complexation but also stabilizes the ICl intermediate and regulates the I-Cl bonding strength to facilitate the subsequent conversion to I2 at the iodine cathode, thereby overcoming the key kinetic bottleneck of the I0/I+ redox process. Simultaneously, Ch+ facilitates Zn2+ transfer kinetics and inhibits water activity, effectively promoting uniform Zn plating with suppressed side reactions. Benefitting from these advantages, the ZIBs assembled with dilute ChCl deliver a high specific capacity of 445 mA h g-1 at 1 A g-1 and achieve 75% capacity retention after 50 000 cycles at a high current density of 10 A g-1. This work provides a facile strategy to simultaneously address the thermodynamic and kinetic issues to enable high-performance four-electron ZIBs.

Light-mediated electronic spin modulation possesses intriguing potentials for photochemistry, enabling on-demand customization of catalysts towards distinct reactions and catalytic requirements. However, the significant photobleaching of the transient spin transitions as well as their temporal mismatch with slower chemical reaction dynamics substantially hinders its applicability. Herein, we demonstrate light-driven steady-state and on-demand catalyst spin modulation that effectively activates plasmonic catalysis. The rapidly oscillating plasmonic electromagnetic near-field spin-polarizes a low-spin CoFe2O4 catalyst and overcomes the photobleaching to produce stable high-spin states with astounding spin lifetimes >60 μs. The high-spin plasmonic catalyst effectively balances the tradeoff between spin polarization and carrier dynamics. For benchmark light-driven nitrate reduction catalysis, it achieves substantial photo-enhancement in ammonia production rate and selectivity as well as photocatalytic performance driven by sunlight, benefiting from polarization activation of nitrate reactant and preferential reaction pathway modulation. The highly generalized light-mediated strategy opens intriguing new avenues for on-demand and steady-state electronic spin engineering with profound implications for distinct disciplines.

Constructing in-plane cationic ordering in layered oxide cathodes can mitigate the adverse effects associated with the anionic redox reaction to achieve high energy density, while recent studies reveal that cationic disordering may also stabilize oxygen redox by tuning the local coordination environment of lattice oxygen. These findings underscore the pivotal role of local coordination and raise a further question regarding how the structural evolution of the transition metal sequence during electrochemical cycling dynamically dictates the charge compensation pathway. Herein, we unraveled the charge compensation evolution of P2-type Na0.6Li0.2Mn0.8O2 (NLMO) upon cationic ordering-disordering transition. During the initial cycle process, the electron holes are delocalized over oxygen ions coordinated to two Mn (O-Mn2) units arranged in the ribbon superstructure within the TM layers of NLMO, enabling a reversible anionic redox reaction. Upon extended cycles, the irreversible chemical depletion of Li and O serves as the thermodynamic driving force that destabilizes the ribbon superstructure. This structural instability facilitates in-plane Mn migration as a kinetic pathway, converting O-Mn2 units to O-Mn3 configurations and driving the macroscopic ordering-to-disordering transition. This fundamental structural disordering uniquely activates the bulk Mn2+/Mn3+ redox couple, which compensates for the diminished anionic redox contribution. By revealing the dynamic coupling between superstructure evolution and redox behavior, this work identifies irreversible cationic transitions as the root cause of structural degradation, underscoring the necessity of constructing rigid TM frameworks in high-capacity layered cathodes.

Constructing electrocatalysts with heterostructures has emerged as an efficient approach to cooperatively catalyze the conversion of lithium polysulfides (LiPSs) in lithium-sulfur (Li-S) batteries. However, it remains a formidable challenge to fundamentally understand the structure-activity relationship between the interfacial configuration and electrocatalytic performance, which is crucial for the rational design of electrocatalysts with heterojunctions. Herein, by leveraging molybdenum carbides (MoxC) with tunable crystal structures as model electrocatalysts, we systematically investigated the geometric-configuration-dependent catalytic activity for LiPS conversion. Experimental analyses confirmed that the cubic MoC with octahedrally coordinated Mo atoms (Mooct) is easily passivated because of its robust LiPS affinity, while the hexagonal Mo2C with triangularly coordinated Mo atoms (Motri) functions better in improving the interfacial charge transfer. Accordingly, the constructed heterointerfaces integrated with dual-geometric coordination endow MoC/Mo2C with moderate LiPS adsorption and favorable charge transfer kinetics to cooperatively catalyze LiPS conversion. Benefiting from these advantages, the Li-S batteries assembled with MoC/Mo2C demonstrate superior reversible specific capacities and cycling durability. This work highlights the critical role of interfacial geometric coordination in heterojunctions for LiPS retention and catalysis, offering a guiding approach for elevating the activity of heterojunction electrocatalysts.

Abstract Composite solid polymer electrolytes (CSPEs) have emerged as promising candidates for next-generation lithium metal batteries. However, the spatial evolution of the solid electrolyte interphase (SEI) at solid-state interfaces remains poorly understood despite its critical role in lithium metal stability. Herein, the anion-trapping layered double hydroxide (LDH) is introduced to poly(ethylene oxide)-based CSPEs to regulate Li+ transport and stabilize the lithium/electrolyte interface. The LDH-enhanced electrolyte achieves exceptional cycling stability over 950 h with a lithium electrode and 90.1% capacity retention after 250 cycles in LiFePO4||Li full cells. Operando nano-focus wide-angle X-ray scattering maps the spatial distributions of both the SEI and lithium dendrites at the lithium/electrolyte interface across micron-scale lateral and vertical dimensions. The regulated Li+ flux promotes homogeneous lithium deposition and the formation of a robust, multifunctional SEI, thereby suppressing lithium dendrite growth and stabilizing the interface. This study provides direct visualization of SEI evolution in CSPEs and clarifies its role in dendrite-free all-solid-state lithium metal batteries.

Abstract Solar-driven chlorine and hydrogen co-evolution from seawater represents an energy-conservating and clean alternative to the conventional chlor-alkali industry. However, sustained and selective chlorine production remains extremely challenging due to competition from the thermodynamically less demanding water oxidation side reaction. In this work, we demonstrate a Ni/Ni2SiO4 plasmonic matrix catalyst that enables a distinct energetic charge carrier filter effect for wavelength-controlled selective chlorine and hydrogen co-production. Based on the distinct energy band structure, the plasmonic-mediated energetic charge filter drives the extraction of higher-energy “hot” holes and lower-energy “cold” electrons, respectively, through lower- and higher-wavelength photons. This phenomenon, combined with hierarchical plasmon coupling and promoted carrier dynamics, collectively led to the cooperative facilitation of both the oxidative and reducing half reactions. In situ spectroscopic investigations point at preferentially promoted chloride adsorption and activation via a two-step, nonradical chlorine evolution pathway, leading to favorable Cl2 and H2 yield rates with near-unity Cl2 selectivity in photocatalytic measurements with seawater. The plasmon-mediated energetic charge carrier filter mechanism opens intriguing pathways for preferential reaction engineering with effective product control.

Aqueous four-electron zinc-iodine (Zn-I2) batteries are appealing next-generation energy storage systems because of their high theoretical energy density, but face critical challenges of parasitic I+ hydrolysis and sluggish iodine redox kinetics. Here, we propose a competitive coordination strategy to address these issues by introducing an ionic liquid-based electrolyte additive comprising chloride anions (Cl-) and 1,3-dimethylimidazolium cations ([DMIm]+). Combined in situ X-ray absorption spectroscopy characterizations and theoretical simulations disclose that the introduced Cl- anions selectively coordinate with electrogenerated I+ species via I-Cl interactions, which partially displace the nucleophilic H2O molecules from iodine solvation shells to suppress the I+ hydrolysis and simultaneously reduce the iodine redox activation barriers. Concurrently, [DMIm]+ cations disrupt the hydrogen bond networks of free H2O molecules through [DMIm]+-H2O coordinations that surpass the strength of intrinsic H2O-H2O hydrogen bonds, effectively passivating the residual H2O activity and mitigating the I+ hydrolysis pathways. Because of these advantages, reversible four-electron iodine redox (I-/I2/I+) is achieved with a close-to-theoretical specific capacity of 405.2 mAh g-1 at 1 A g-1 accompanied with a low fading rate of 0.00058% per cycle over 60,000 cycles at 10 A g-1. This work establishes a promising avenue to achieve stable four-electron redox chemistry for practical aqueous Zn-I2 batteries.

O3-type nickel-manganese-based layered cathodes are appealing for building high-energy sodium-ion batteries (SIBs) in growing energy storage application. However, the complicated phase transitions and sluggish Na+ kinetics have largely impeded their practical applications. Herein, this work proposes a medium-entropy strategy for O3-type NaNi0.5Mn0.5O2 cathode to regulate the covalency of Ni/Mn-O bonds via reinforcing TM-O bonding strength, which leads to the contraction of d (O-TM-O) and elongation of d (O-Na-O). Experimental analysis combined with theoretical calculations verifies that the entropy regulation contributes to the retention of O3-type structure and suppressed excessive TM slab gliding and stabilizes Na+ migration pathways as well as limited precipitation of high-valent Ni ions during the cyclic process. Consequently, the designed O3-Na0.92Ni0.47Nb0.03Mn0.30Ti0.20O2 (NNNMTO) demonstrates an excellent rate capability (53 mAh g-1 at 10 C) and long-term cycling stability (70% capacity retention at 2 C after 500 cycles) under a wide working voltage range between 2.0-4.2 V, along with less moisture sensitivity. Additionally, the full battery paired with commercial hard carbon anode displays an impressive cycling stability with an energy density of 260 Wh kg-1 based on the active material mass of both electrodes, making its practical operation possible. This work provides insightful perspectives in facilitating Na+ diffusion and mitigating the undesirable phase transition for layered oxide cathode materials of high-energy SIBs.

With the increasing prevalence of antibiotic-resistant bacteria, the effectiveness of traditional antibiotics in treating bacterial infections has diminished. To address this challenge, we developed a bilayer hydrogel with sustained antibacterial activity that can efficiently load clove essential oil. The lower layer consists of a polyvinyl alcohol (PVA) hydrogel combined with copper nanosheets (CuNSs), while the upper layer is a mixture of PVA and polyethylene glycol incorporated with essential oil (EO). CuNSs initially exert antibacterial effects by gradually releasing Cu2+ ions. At the same time, EO provides effective antibacterial action and hydrophobicity, ensuring prolonged bacterial inhibition through slow release. In vitro bacterial inhibition experiments indicated that the bilayer hydrogel maintained 96% antibacterial efficacy even after 72 h. Furthermore, the bilayer hydrogel exhibited superior mechanical strength, solubility, water retention, and thermal stability compared to monolayer hydrogels. These findings suggest that the bilayer hydrogel holds great potential for long-term infection control applications.

The widespread use of tetracycline (TC) has resulted in severe water pollution, highlighting the urgent need for efficient degradation technologies. In this study, a Bi-BTC/BiYO 3 /CA photocatalyst was synthesized using cellulose acetate (CA) as a carrier via a solvothermal process combined with nonsolvent-induced phase separation, and its photocatalytic performance in TC degradation was systematically evaluated. Under optimal conditions, a degradation efficiency of 95.06% was achieved. Both experimental and theoretical analyses revealed that the formation of the Bi-BTC/BiYO 3 heterojunction enhances the separation of photogenerated charge carriers and improves visible-light absorption, whereas the incorporation of CA significantly boosts the material's recyclability. Various characterization methods confirmed the successful synthesis of Bi-BTC/BiYO 3 /CA. Additionally, the efficient carrier separation and expansion of the light absorption range achieved by the Bi-BTC/BiYO 3 heterojunction were demonstrated. Notably, the photocatalyst retained 91% of its initial degradation efficiency after four recycling cycles, underscoring the potential of the CA-based composite catalyst for application in simulated wastewater treatment. This synergistic integration of a heterojunction and carrier provides a promising strategy for the effective degradation of environmental pollutants.

Fast-charging capabilities of sodium-ion batteries have emerged as a pivotal objective within the energy storage fields. Sodium layered P2-type oxide positive electrodes are considered promising for fast charging due to their inherent fast Na+ mobility. However, their electrochemical polarization and interfacial charge transfer especially at high state of charge are limiting factors in quick kinetic response for large current. Herein, we demonstrate that a typical P2-type positive electrode (Na0.7Ni0.27Mn0.53Cu0.04Fe0.08Ti0.08O2) achieves high-rate capacities through avoiding octahedral stacking faults, maintaining lattice oxygen activity and controlling anion-specific adsorption. The intermediate Z-phase intergrowth structure mitigates kinetic polarization and thermodynamic hysteresis by simultaneously suppressing the unfavorable phase evolution from P2-type to O2-type and irreversible oxygen redox. The potential-dependent competitive adsorption mechanism between anions and solvent molecules is revealed within the inner Helmholtz plane, where optimized anion-specific adsorption elevates potential difference between electrodes and inner Helmholtz plane, accelerating charge transfer across the electrode/electrolyte interface. Furthermore, the F-rich cathode/electrolyte interphase generated from inner Helmholtz plane mitigates transition metal dissolution and surface lattice collapse for stable long-term cycling. This study highlights the synergistic coupling interaction between bulk phase stability and interfacial environment optimization in ensuring fast Na+/charge transport kinetics for sodium-ion batteries.

Lattice-oxygen redox in layered oxides can enhance energy density, but its limited reversibility causes structural instability during deep cycling. Here we develop an iron-mediated strategy to regulate lattice-oxygen redox in layered oxide cathodes. In the Na2/3Mn7/12Mg1/4Fe1/6O2 cathode, Fe ions act as redox mediators, with Fe4+ capturing electrons from lattice oxygen during charging and Fe2+ donating electrons back to oxidized oxygen during discharging through chemical pathways. With the assistance of iron mediation, the reversibility of lattice-oxygen redox is dramatically improved from 75% to 99%. As a result, the lattice-oxygen-activated cathode enables a sodium-ion pouch cell to achieve an energy density of 206 Wh kg−1 and operate stably for 100 cycles at 50 mA g−1, with a capacity retention of 87.8%. Lattice-oxygen redox can raise the energy density of layered oxide cathodes, but poor reversibility causes structural degradation and capacity loss. Here the authors use iron as a bulk redox mediator to boost oxygen-redox reversibility and stabilize high-energy sodium-ion batteries.

Catalytic conversion of lithium polysulfides (LiPSs) is a promising avenue to suppress the shuttle effect and enhance the redox kinetics of lithium–sulfur (Li–S) batteries. However, the consecutive multiple LiPSs redox reactions make the activity prediction of electrocatalysts elusive. Herein, we propose a lower Hubbard band (LHB) descriptor to regulate tandem electrocatalytic LiPSs conversion for fast and robust Li–S batteries. Combined with theoretical calculations, the catalytic activity is jointly determined by the balance between LHB center position (ƐLHB) and LHB width (ꞶLHB). As a proof of concept, Fe3O4@FeP shows a balance of possessing a close ƐLHB to the Fermi level and a wide ꞶLHB simultaneously. An accelerated tandem electrocatalytic LiPSs conversion is achieved, where a close ƐLHB to Fermi level (with Fe3O4 as the active center) benefits the adsorption of long-chain LiPSs and catalyzes S8-to-Li2S4 process, while a wide ꞶLHB (with FeP as the active center) subsequently contributes to catalyze the Li2S4-to-Li2S reaction. Consequently, the elaborate Li–S batteries deliver outstanding cycle stability over 1000 cycles and superior rate performance over 10 C. Further, the constructed Ah-scale pouch cell delivers notable energy density of 360.6 Wh kg−1. This work demonstrates the great promise of LHB regulation strategy for designing high-efficient electrocatalysts for Li–S batteries and beyond.

Ion exchange provides a versatile route to access metastable layered oxide materials beyond conventional thermodynamic limits, yet its development has been constrained by an insufficient understanding of how synthesis pathways govern exchange kinetics, structural evolution, and electrochemical performance. Using Na0.6Li0.2Mn0.8O2─a P2-type cathode for sodium-ion batteries─as a well-defined model, we uncover how distinct ion-exchange methods─solid-state ball milling and liquid-phase ultrasonication─induce fundamentally different exchange behaviors via distinct energy-transfer modes. Ball milling drives rapid defect-mediated exchange and a stress-activated 1/5 → 1/3 superstructure transition. In contrast, ultrasonication leads to kinetically limited exchange with intralayer disorder through a collective phonon-like mechanism. Atomic-scale imaging reveals that these contrasting modes give rise to distinct interlayer slip dynamics: short-range stress-driven slip in ball-milled samples and long-range cooperative slip under ultrasonication, both propagating layerwise along aligned ion-diffusion channels. Guided by these mechanistic insights, we develop a sequential ball milling-ultrasonication process that achieves near-complete exchange (98.3 %) within 2 h while retaining the structural integrity. Subsequent postannealing repairs defects and yields a cathode with a reversible capacity of 235 mAh/g (versus lithium metal). This work establishes a rational design framework for efficient, structure-preserving cathode synthesis and reveals general principles governing ion-exchange chemistry in solid oxides.

Silicon monoxide (SiO) is a promising anode material for next-generation lithium-ion batteries, yet the practical application remains hindered by drastic volume expansion, unstable solid electrolyte interphase (SEI), and sluggish reaction kinetics. Herein, we propose a rational interfacial engineering strategy to construct a robust O–Fe–C bridging architecture for SiO via high-energy ball-milling combined with in situ polymerization and carbonization. It has been demonstrated that the constructed O–Fe–C architecture establishes a highly efficient electron/ion transport network to significantly accelerate charge transfer kinetics. More importantly, such bridging structure could also function as an elastic buffer with a distinctive “spring effect” to accommodate the volume expansion of SiO over cycling, which effectively suppresses the interfacial rupture and regulates the electrolyte decomposition to foster a stable and LiF-rich SEI layer. Consequently, the SiO anode with the O–Fe–C bridging architecture delivers a superior reversible capacity of 1061.4 mA h g−1 after 100 cycles at 0.1 A g−1, and a high rate capability of 613.0 mA h g−1 at 3.0 A g−1. This work offers deeper insights into interfacial design for stable silicon-based anodes with enhanced reaction kinetics, providing a feasible strategy for the construction of next-generation energy storage systems.