Phosphate rock resources, which are of high strategic importance and facing increasing demand, urgently require the development of a low-carbon and sustainable phosphorus recovery process to address current limitations. In this study, a novel photoelectrically driven electrochemical struvite electrolyzer was developed using electrode oxidation, with simulated swine wastewater as the research medium. Four distinct influencing conditions were examined to evaluate their impact on the phosphorus recovery efficiency and the characteristics of the recovered struvite product. Furthermore, the optimal conditions were validated using actual swine wastewater. The experimental results indicated that, under the optimal influencing conditions (flow rate of 20 L/h, current density of 144.3 A/m2 and electrode spacing of 3.5 cm), the phosphate concentration in the actual wastewater was reduced from 215 +/- 15 mg/L to 2.1 +/- 0.5 mg/L, achieving a phosphorus recovery rate of 99.3 %. Characterization analyses revealed that the struvite synthesized under the optimal influencing conditions possessed an orthorhombic crystal structure with high crystallinity. An economic feasibility assessment revealed that the cost of treating actual swine wastewater using this method was estimated at $18.88/kgPO4-P and a solar energy overproduction rate of 226 % during full-scale operation. Therefore, this method has substantial economic and environmental benefits. This study demonstrated a promising strategy for integrating electrode oxidation into a photovoltaic-driven struvite electrolytic cell for phosphorus recovery. The approach used provides a novel technological pathway for the sustainable and low-carbon recovery of phosphorus from diverse wastewater streams, contributing to the development of a circular economy.

Zinc metal anodes (ZMAs) in aqueous zinc-ion batteries are hindered by parasitic reactions arising from unstable electrolyte pH, low Zn2* transport number, and limited ionic conductivity, which critically restrict cycling stability and practical applicability. Here, we propose a high-entropy electrolyte paradigm based on molecular diversity, in which six structurally distinct amino acids are simultaneously incorporated into a ZnSO4 electrolyte to construct an amino acid-based high-entropy electrolyte (AA-HEE). Spectroscopic characterizations combined with molecular dynamics simulations provide direct evidence that the AA-HEE reaches a high-entropy state. Benefiting from the synergistic interactions among multiple amino acids, the AA-HEE exhibits a unique Zn2* solvation structure featuring both direct coordination and indirect stabilization of the hydrogen-bond network. Consequently, the chemical and electrochemical stability of the ZMAs|AA-HEE interface, together with the ion transport kinetics of the electrolyte, are substantially enhanced. As a result, ZMAs with effectively suppressed dendrites, HER, and passivation are achieved. The AA-HEE enabled Zn||Zn symmetric cells cycle stably for over 5300 hat 1 mA cm-2, while Zn||NH4V4O10 full cells deliver 82.9% capacity retention after 1500 cycles at 5 A g-1 and exhibit outstanding rate capability and low self-discharge ratio. These results highlight high-entropy electrolyte engineering as an effective strategy for high-performance aqueous zinc-ion batteries. (c) 2026 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 integration of surface-regular micro/nanostructured electrodes within a limited footprint area is promising to enhance the electrochemical performance of planar micro-supercapacitors (P-MSCs), while developing simple yet efficient manufacturing methods for such electrodes remains a challenge. Here, we propose a universal strategy combining femtosecond laser plasma lithography with spatial light modulation (SLM-FPL), fabricating well-ordered sub-wavelength micro/nanostructured electrodes of interdigital P-MSCs (SEP-MSCs) on graphene oxide (GO) films. Achieving 500/50 µm finger widths/spacings and 680 nm internal grating periods, this method enables device densities >25 units inch−2 with processing efficiency orders of magnitude higher than conventional laser direct writing. Further performance optimizations via wettability modification, electric field engineering, and hybrid composites (GO-MXene/COF) yield outstanding specific capacitance ( 41.4 F cm−3) and cycling stability (93

Polyanionic cathode materials based on Mn/V redox couples offer high-voltage plateaux and high theoretical energy density for sodium-ion batteries (SIBs). However, they suffer from severe degradation in rate capability and cycling stability under high-voltage, whose microscopic origin remains elusive on the electronic-level. Herein, we reveal the strong coupling between Mn/V-O antibonding orbitals at elevated voltages induces significant lattice strain, leading to kinetic hysteresis. Thus, we propose a targeted orbital engineering regulation strategy aiming to disentangle the strong coupling among (TM-O)* orbitals. By introducing Ti4+ (3d0) and Fe3+ (3d5) as the stable electronic configurations, and electron-donating Si, we modulate (TM-O)* orbital occupancy at the electronic level, markedly alleviating structural stress and stabilizing Na+ diffusion pathways. The optimized Na4Mn0.7V0.7Ti0.4Fe0.2(PO4)2.9(SiO4)0.1 cathode delivers high energy density (415.03 Wh/kg) and exceptional long-cycle performance, retaining 80.3% capacity after 8,000 cycles at 20 C. This strategy demonstrates a feasible orbital engineering approach to develop stable high-energy-density cathodes for SIBs.

Na4VMn(PO4)3, as a high-energy-density and low-cost cathode material for sodium-ion batteries (SIBs), holds promising application prospects. However, its practical performance is limited by the stepwise redox reactions of V and Mn, which induce significant phase transitions and sluggish kinetics, particularly during the second desodiation process. To address this issue, we propose an orbital hybridization regulation strategy based on Ti/Fe co-doping. By tailoring the local coordination environment, the introduced Ti/Fe constructs a 3d-3d metallic network, inducing continuous multi-orbital hybridization. This transforms the V/Mn redox process from stepwise to simultaneous, eliminating sharp phase boundaries and overcoming the kinetic bottleneck in the second desodiation step. Additionally, the d-band energy level difference between V and Mn is narrowed to 0.701 eV, enhancing electron delocalization and intrinsic conductivity, thereby enabling highly reversible multi-electron transfer processes. The optimized Na3.75V0.75Mn0.75Ti0.25Fe0.25(PO4)3 effectively mitigates volumetric stress and local phase transitions, ensuring structural integrity. Consequently, the material retains 73% capacity after 2000 cycles at 10C, demonstrating superior rate capability and cycling stability. This work provides crucial electronic-level insights and a novel design paradigm for high-performance SIB cathode materials.

Conventional coal pyrolysis tends to drive aromatic condensation and graphitic stacking, which limits closed-pore formation and leads to sluggish Na+ transport, low plateau capacity and poor initial Coulombic efficiency (ICE) in coal-derived hard carbon. Here we develop a rapid temperature shock (RTS) strategy to redirect coal carbonization through a kinetically constrained thermal pathway. The rapid heating restrains graphitic rearrangement and secondary condensation, while promoting cross-linked disordered carbon reconstruction. The resulting RTS-HC exhibits an enlarged d002 spacing of 0.392 nm, abundant closed nanopores and a turbostratic carbon framework. These structural features lower the Na+ migration barrier to 0.38 eV and facilitate reversible low-potential Na storage. Density functional theory calculations further indicate that confined Na-carbon interactions with partial ionic character stabilize Na storage within closed pores. As a result, RTS-HC delivers a reversible capacity of 303.6 mAh g-1 at 30 mA g-1, a high ICE of 89% and a plateau contribution of 67%. It also retains 80.4% of its capacity after 1000 cycles at 500 mA g-1, outperforming the conventionally pyrolyzed counterpart. This work provides a kinetic carbonization strategy for converting coal into high-performance hard carbon anodes for sodium-ion batteries.

ABSTRACT Sustainable aqueous zinc‐ion batteries (AZIBs) have emerged as promising next‐generation energy storage solutions, aligning with global initiatives to mitigate climate change and promote low‐carbon transitions. Their appeal stems from the utilization of earth‐abundant materials and aqueous electrolytes, which minimize reliance on scarce metals and alleviate the safety and environmental risks associated with organic‐solvent‐based systems. This review systematically evaluates the sustainability of AZIBs throughout their entire life cycle, encompassing material selection, cell manufacturing, operational use, and end‐of‐life recycling, while providing a forward‐looking perspective on their advancement. However, critical hurdles to industrialization persist, including zinc dendrite growth, cathode dissolution, and restricted cycle life. To realize genuine sustainability, future research must prioritize green material innovations, such as bio‐based binders, functional separators, and eco‐friendly electrolytes, while implementing dry electrode fabrication and other low‐impact manufacturing techniques. Adopting a comprehensive life‐cycle approach guided by circular economy principles is vital for fostering synergistic optimization across design, production, use, and recycling, ultimately achieving a “cradle‐to‐cradle” system. Furthermore, supportive policies, cross‐sector collaboration, and international standardization are essential to bridge the gap between laboratory research and large‐scale application. Through systematic, multi‐faceted innovation, sustainable AZIBs are well‐positioned to drive the global energy transition.

The rational design of high-entropy materials for electrochemical energy storage is hindered by an insufficient understanding of the distinct roles of constituent elements. Taking the spinel-type high-entropy oxide (CoCuMgCrFe)3O4 as a model system, this study combines density functional theory calculations with multiscale characterization to systematically reveal the functional differentiation mechanism of the constituent elements during charge/discharge processes. It is demonstrated that Cr, Co, and Fe act as "active elements" significantly enhancing the decomposition kinetics of Li2O, while Cu and Mg serve as "structural elements" effectively suppressing volume expansion induced by lithium intercalation, thereby improving structural stability. Critically, all high-entropy surfaces exhibit exceptionally strong adsorption of Li2O intermediates (adsorption energy: -5.35 to -5.64 eV), which is attributed to the synergistic modulation of the electronic structure within the high-entropy environment, thereby accelerating conversion reactions. Bond length analysis identifies the weakening of Li-O bonds near active sites, with Cr exerting the most profound influence. Furthermore, we establish the metal-oxygen bonding radius as a critical descriptor for predicting high-entropy spinel formation. This work unveils the fundamental principle of elemental cooperation in high-entropy oxides, providing crucial guidance for the targeted design of high-performance multicomponent electrodes.

As a sustainable cathode material for sodium-ion batteries, Na4MnFe(PO4)3 (NMFP) is prized for high theoretical operating voltage and cost-effectiveness. However, its practical electrochemical activity is notoriously poor, contradicting theoretical predictions. Here, we reveal that this inactivity stems primarily from Mott localization, driven by strong electron correlations within the high-spin 3d5 electronic configuration (t2g 3eg 2) of Mn2+ and Fe3+. This symmetric, half-filled state leads to pronounced charge localization, severely suppressing the intrinsic redox activity. To address this limitation, we devised a symmetry-breaking reconstruction strategy which reorganizes the spin ordering to promote electron delocalization and activates multiple redox couples (Mn4+/Mn3+, Mn3+/Mn2+, and Fe3+/Fe2+). More critically, induce a novel "Na2 dp Na1" migration path for Na+, with a remarkably lower energy barrier than those of conventional paths (0.39 vs. 0.98 eV). Consequently, the engineered Na4Mn0.5Fe0.5Cr0.5Ti0.5(PO4)3 delivers 138.84 mAh g-1 at 0.1C, which represents a 12.74-fold breakthrough over the pristine NMFP (10.9 mAh g-1). Our findings elucidate symmetry-breaking as a critical route for activating Mott-localized states in polyanionic frameworks and establish a new paradigm for designing redox-active and sustainable cathode materials.

High-voltage and high-temperature sodium-ion batteries (SIBs) promise cost-effective energy storage applications in extreme scenarios, but a critical dilemma persists: the chemical and electrochemical instability of conventional electrolytes. The intensified electrolyte consumption, electrode failure, and interface damage result from aggressive H+ corrosion, especially in NaPF6-based electrolytes. To address this challenge, this study proposes a molecular design strategy based on an asymmetric glycol-ether (F3Si) cosolvent. Leveraging its steric hindrance effect, we modulate the Na+ coordination environment, thereby altering traditional solvation structures and promoting anion participation in constructing a stable, inorganic-rich cathode-electrolyte interphase (CEI). Experimental and theoretical simulation results demonstrate that the involvement of F3Si in the Na+ solvation sheath exhibits temperature-adaptive characteristics: as temperature increases, more anions are incorporated into the coordination sphere, facilitating the formation of a high-modulus, inorganic-rich CEI. Meanwhile, the F3Si cosolvent effectively captures adverse acidic species via Si-O bonding, interrupting subsequent chain-like side reactions. Consequently, the developed electrolyte enables the 4.3 V-Na3V2(PO4)2O2F cathode to demonstrate exceptional cycling stability under extreme thermal conditions─retaining 88.9% of capacity after 2000 cycles at 70 °C and maintaining 98.5% of capacity over 400 cycles at 90 °C. This work elucidates a temperature-responsive interface stabilization mechanism rooted in solvent molecular geometry and anion solvation, offering innovative electrolyte design principles for developing high-performance SIBs in harsh temperature regimes.

Polyanionic Na3VCr(PO4)3 is a promising high-voltage cathode for sodium-ion batteries, yet it suffers from severe interfacial degradation at deep desodiation, including transition metal dissolution, irreversible phase transitions, and side reactions, especially under extreme temperatures. To overcome this, we design a graphitized topological interface-a 3D continuous graphitized network coating the material particles. This interface not only enhances electron/ion transport but also templates the formation of a thin, uniform, and inorganic-rich cathode electrolyte interphase (CEI) via selective electrolyte adsorption, shifting CEI growth from passive blocking to active induction. Moreover, it suppresses transition metal leaching and mitigates lattice distortion, thereby stabilizing the bulk structure. With such dual stabilization, the modified cathode exhibits superior wide-temperature performance: retaining 70.3% after 1000 cycles at room temperature, while delivering capacities of 69.6 mAh g-1 (74.3% capacity retention) and 86.1 mAh g-1 at -40 degrees C and 50 degrees C, respectively, with excellent cycling durability. This work provides a new paradigm for high-energy cathode design.

Aqueous zinc-iodine batteries(Zn-I2Bs)emerge as promising candidates for grid-scale energy storage due to their inherent safety,low cost,and environmental benignity.However,their practical deployment is hindered by critical challenges,including severe self-discharge driven by coupled polyiodide shutting and hydrogen evolution reaction(HER),limited practical energy density constrained by low voltage plateaus and predominantly two-electron iodine redox,sluggish reaction kinetics from complex iodine species interconversion,and zinc anode instability(dendrites,corrosion,passivation).This work provides a comprehensive analysis of Zn-I2B mechanisms,debating the interplay between iodine's layered structure favoring intercalation and its multivalency enabling conversion reactions,particularly pathways for electron redox beyond I-/I2.Strategies to mitigate these challenges are critically reviewed:anchoring iodine species within tailored host materials(e.g.,functionalized carbons,COFs,perovskites)to suppress shuttling;electrolyte engineering(e.g.,DES,additives)to sequester free I-and modulate solvation;functional separators/membranes for ion sieving;catalytic materials(transition metal/nonmetal-based)to accelerate kinetics;and anode protection/modification(interfacial layers,hydrogel electrolytes,nonmetallic anodes)to enhance reversibility.The review synthesizes recent advances,identifies persistent bottlenecks,and outlines future research directions essential for realizing the commercial potential of high-performance Zn-I2Bs.

Lithium demand is rapidly increasing due to the expansion of electric vehicles and large-scale energy storage systems. Salt lake brines contain approximately 65% of the world's lithium resources and represent an important source for lithium production, particularly for countries such as China with high import dependence. However, the complex composition of salt lake brines and the significant variability among different brine resources pose substantial challenges to efficient lithium recovery. In particular, some salt lake brines exhibit high Mg/Li ratios, making Mg/Li separation one of the major technical barriers to lithium extraction. This review systematically summarizes recent advances in lithium extraction technologies for high Mg/Li ratio salt lake brines, with a focus on direct lithium extraction (DLE) approaches, including adsorption, membrane separation, solvent extraction, and electrochemical methods. The separation mechanisms, recent research progress, advantages, limitations, and industrialization status of these technologies are critically discussed. Particular attention is given to three major classes of inorganic lithium adsorbents, namely manganese-based, titanium-based, and aluminum-based materials, with a comparative analysis of their structural characteristics, lithium selectivity, and extraction performance. Powder adsorbents suffer from inherent drawbacks such as poor mechanical strength, low flowability, and insufficient permeability, which severely hinder their direct industrial application. Recent developments in shaping technologies for powder adsorbents are thus summarized including granulation, membrane fabrication, and foam structuring. Finally, the key challenges and future prospects for lithium extraction from salt lake brines are discussed, aiming to provide insights for the efficient, sustainable, and large-scale utilization of salt lake lithium resources.

Quinone-based electrode materials hold significant promise for next-generation sodium-ion batteries due to their structurally tailorable frameworks, high theoretical capacities, and favorable redox potentials. However, dissolution in organic electrolytes and structural instability during cycling critically impair their capacity retention and cycling durability. Herein, we designed and synthesized two novel acylimide materials N , N '-bis(2,6-anthraquinone diamine)-biphenyl diimide (DQ-BDI) and N , N '-bis(anthraquinone-2,6diamine)-perylenyl diimide (DQ-PDI) with the gradual enhancement of 7r-conjugation. Electrochemical characterization reveals exceptional performance in DQ-PDI. At the current density of 50 mA/g, the DQPDI delivered the first discharge specific capacity of 158 mAh/g, and the capacity retention of 99 % after 100 cycles, with the coulombic efficiency of nearly 100 %. At a high current density of 500 mA/g, the DQPDI displays a high discharge capacity of 152 mAh/g. The reduction peaks of DQ-PDI located at 2.28 V and 1.34 V are the insertion reactions of sodium ion from the carbonyl groups on PTCDA unit and on DAAQ unit at both ends, respectively, and the two oxidation peaks at 2.58 V and 1.53 V corresponds to extraction reactions. Compared with DQ-BDI, DQ-PDI exhibits a larger 7r-conjugation plane, which significantly enhances the intermolecular 7r- 7r interactions. It can well reduce the dissolution of the material in organic electrolyte, resulting in a higher discharge capacity, superior cycling stability and accelerated reaction kinetics. Our 7r-conjugation extension strategy establishes a new paradigm for designing dissolution-resistant, high-performance organic electrodes. (c) 2026 Published by Elsevier B.V. on behalf of Chinese Chemical Society and Institute of Materia Medica, Chinese Academy of Medical Sciences.

Carbon-based materials have emerged as promising anodes for potassium-ion batteries (PIBs) owing to their natural abundance, structural stability, and tunable architectures. However, the repeated intercalation/deintercalation of large-size K+ induces anode materials structural collapse and severe volume expansion, and consequently, leading to rapid capacity fading and poor cycling stability. To address these challenges, we designed sulfur/nitrogen co-doped porous carbon (S/N, PCs-900) with engineered edge defects and abundant electroactive sites, significantly enhancing its electrochemical performance. The optimized S/N, PCs-900 anode delivers exceptional reversible capacity (420.8 mAh g- 1 at 0.1 A g- 1 over 500 cycles) and ultralong cycle life (215 mAh g- 1 at 5 A g- 1 after 5000 cycles), outperforming most reported carbonaceous PIB anodes. Furthermore, this work elucidates the critical role of heteroatom co-doping in enabling fast and stable potassium storage, providing a universal strategy for advancing high-performance energy storage materials.

The implementation of sodium metal anodes (SMAs) is critically hindered by dendritic growth and interfacial instability, challenges that become particularly severe at low temperatures due to sluggish ion transport and increased interfacial resistance. To address this, a novel heterojunction artificial interphase comprising Na3Sb and Na2Te is constructed in situ on the sodium metal surface. This unique architecture exhibits a remarkable synergistic effect from the dual components. Specifically, the highly sodiophilic Na3Sb alloy phase offers superior mechanical properties and effective sodium anchoring sites, which adequately guide the uniform deposition of sodium, thereby enabling a highly stable and dendrite-free sodium metal anode. Simultaneously, the Na2Te component, as an excellent electronic conductor, establishes an efficient electron transport network, drastically lowering the charge-transfer resistance and accelerating interfacial reaction kinetics. Benefiting from this rational design, the symmetric cell achieves an extended cycling lifetime of 2100 h (0.5 mA cm-2/1.0 mAh cm-2). More impressively, full cells paired with a Na3V2(PO4)3 cathode demonstrate exceptional cycling durability, retaining 4000 cycles at 5 C (25 degrees C) and 1100 cycles at 4 C even under an ultra-low temperature of -40 degrees C. This work provides a strategic design of a multifunctional interphase for durable SMAs operable across a wide temperature range.

Na4MnV(PO4)3 stands as a promising cathode material for sodium-ion batteries owing to its low cost and multiple redox potentials. However, challenges such as drastic local distortion, irreversible phase evolution, and transition metal dissolution in multielectron redox processes, coupled with intrinsic low electronic conductivity jointly trouble its practical deployment. Herein, the Ti4+ with a d0 arrangement is employed to customize the TM-O bonds to eliminate the structural distortion in Na4MnV(PO4)3. The coupling coordination effect of multiple transition metals activates the Mn4+/3+ redox while reinforcing structural stability in over two-electron redox processes, enabling the Na3.1(MnV)0.7Ti0.6(PO4)3 (MnVTi) cathode to realize a 2.4 e- reversible transfer and deliver a specific capacity of 138.4 mAh g-1. Experimental and theoretical calculations reveal that robust TM-O bonds with dynamic covalent chemistry, particularly the strong covalent Ti-O bonds, unlock ultrafast and durable cycling performance (78.4% capacity retention after 10,000 cycles at 20 C). Furthermore, the enhanced electronic conductivity and reaction kinetics contribute to the exceptional rate performance (74.2 mAh g-1 at 50 C), fast-charging capability (1.77 min to reach 80% SOC), and fabulous all-weather adaptability (-40 to 50 °C). This work establishes a universal design paradigm for high-performance Mn-based polyanion cathodes through d0-metal coupling mediated by dynamic covalent chemistry.

ABSTRACT Na 4 MnV(PO 4 ) 3 , characterized by cost‐effectiveness, high voltage, and tunable chemical structure, has drawn considerable attention. However, the practical deployment is hindered by drastic local structural distortions induced by over two electron transfers, coupled with intrinsically low electronic conductivity. Herein, a Schottky and 3 d ‐orbital coupling design paradigm is performed to synergistically tailor the TM‐O coordination environment and interfacial structures, thus breaking the dual bottlenecks of poor electrode kinetics and structural fragility. Therefore, the prepared Schottky‐orbital coupling mediated Na 4 MnV(PO 4 ) 3 (SOMV) cathode exhibits continuous multistep redox with a reversible discharge capacity of 143.9 mAh g −1 at 0.1 C. Theoretical calculations and experiment demonstrate that the in‐situ generated metallic Ni 2 P particles establish intimate contact with semiconducting phosphate particles, inducing the built‐in electric field and thus facilitating the coupled ion‐electron transfer and elevating the reaction‐limited current. Eventually, the SOMV cathode achieves a remarkable rate (82.5 mAh g −1 at 30 C) and fast‐charging performance (26 s to reach 88.5 mAh g −1 ). Moreover, the multiple TM 3 d ‐orbital coupling and reinforced TM─O bonds of SOMV grant the excellent long‐term cycling stability (75.0% capacity retention after 10 000 cycles at 30 C). A universal paradigm for boosting the coupled ion‐electron transfer is established via synergistic engineering of electronic and structural properties.

The large-scale applications of anion exchange membrane water electrolysis (AEMWEs) and zinc-air batteries (ZABs) are observably limited by the lack of highly active, multifunctional, and industrially applicable electrocatalysts. In this work, we report a solvent-free rapid pyrolysis strategy that successfully prepares a composite material of Pt8V-V2O3 heterostructure supported on nitrogen-doped porous carbon (Pt8V-V2O3@NPC). In alkaline hydrogen evolution reactions, the mass activity of Pt8V-V2O3@NPC reaches 10.6 times that of commercial Pt/C, while the half-wave potential for the oxygen reduction reaction is 0.89 V. The assembled ZABs demonstrate stable cycling performance over 5550 cycles at a current density of 5.0 mA cm-2, with negligible voltage decay. Likewise, AEMWEs incorporating this material exhibit stable operation for over 500 h at a current density of 1000 mA cm-2, with a voltage decay rate of only 0.14 mV h-1. Combined X-ray absorption fine structure spectroscopy and theoretical studies demonstrate that the interfacial electron transfer from V2O3 to Pt8V optimizes the d-band center of Pt8V-V2O3. This study proposes an interface electronic bridging strategy for the design of multifunctional electrocatalysts, which may provide support for the development of practical clean energy technologies.