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Wadsley–Roth phase niobium‐based oxides show potential as anode candidates for fast‐charging lithium‐ion batteries. Traditional synthesis methods, however, usually involve a time‐consuming calcination process, resulting in poor production efficiency. Herein, a novel carbothermal shock (CTS) method that enables the ultra‐fast synthesis of various Wadsley–Roth phase Nb‐based oxides within seconds is introduced. The extremely rapid heating rates enabled by CTS alter the reaction mechanism from a sluggish solid‐state process to a swift liquid‐phase assisted one and drive the chemical reactions away from equilibrium, thereby generating abundant oxygen vacancies and dislocations. Theoretical calculations reveal that oxygen vacancies significantly lower the energy barrier for Li+ diffusion and enhance the intrinsic electronic conductivity. Moreover, dislocations help convert the surface tensile stress arising from Li+ intercalation into compressive stress, effectively improving the structural integrity during cycling. Notably, this approach can also be applied to synthesize LiFePO4 cathode materials under ambient conditions, eliminating the requirement for inert atmospheres. Consequently, the CTS‐synthesized Nb14W3O44||LiFePO4 battery demonstrates reversible structural evolution validated by in situ XRD and exceptional cycling ability (e.g., 0.0065% capacity decay per cycle at 4 A g−1 over 3000 cycles). Importantly, the Nb14W3O44||LiFePO4 configuration also shows enhanced thermal stability in the Ah‐level pouch cell nail penetration test, confirming its feasibility. [ABSTRACT FROM AUTHOR]

Aqueous zinc–iodine (Zn–I2) batteries, with their outstanding merits in safety, cost, and environmental friendliness, have received extensive attention. However, the unstable electrochemistry at the electrode–electrolyte interface originating from free water results in zinc dendrite growth, hydrogen evolution reaction (HER), and polyiodide ions shuttle, hindering their practical applications. Herein, solid‐state Zn–I2 batteries based on an inorganic ZnPS3 (ZPS) electrolyte are developed to overcome inherent interfacial issues associated with aqueous electrolytes. The inorganic ZnPS3 electrolyte, with a low Zn2+ diffusion energy barrier of ≈0.3 eV, demonstrates an exceptional ion conductivity of 2.0 × 10−3 S cm−1 (30 °C), which also satisfies high chemical/electrochemical stability and mechanical strength. The solid Zn2+ conduction mechanism, facilitated by bounded water only on grains, effectively suppresses HER and polyiodide ions shuttling. During cycling, a ZnS functional layer is spontaneously formed on the anode/electrolyte interphase, promoting dendrite‐free Zn deposition behavior with a more stable (002) crystal orientation. Consequently, the solid‐state configuration of Zn–I2 battery enables an impressive reversible capacity of 154.2 mAh g−1 after 400 cycles at 0.1 A g−1. Importantly, the compatibility of the solid‐state ZnPS3 electrolyte is also confirmed in the Zn||CuS cell, indicating its potential as a versatile platform for developing inorganic solid‐state zinc‐ion batteries (ZIBs). [ABSTRACT FROM AUTHOR]

Th all phenyl complex (APC) electrolyte is generally accepted to be compatible with Mg metal anodes, offering excellent plating/stripping reversibility. However, the large Cl desolvation penalty of the MgCl+ solvation structure in APC electrolyte causes a high reaction energy barrier at the cathode/electrolyte interface, resulting in unsatisfactory rate performance. Herein, the interface reconstruction strategy of an anatase TiO2 cathode is proposed by the combination of ultrathin carbon coating and oxygen vacancies, which realizes the fast surface‐redox pseudocapacitance charge storage mechanism via MgCl+, circumventing the sluggish solid‐phase migration of Mg2+. Theoretical calculations verify that the introduction of oxygen vacancies in TiO2, not only increases the intrinsic electronic conductivity, but also improves the adsorption capability for MgCl+, which enhances the surface‐redox pseudocapacitance of TiO2. Moreover, in situ Raman measurements, ex situ XPS spectra and XRD patterns demonstrate the structural integrity of TiO2 without undergoing phase change and the rapid reversible storage of MgCl+. Furthermore, in situ electrochemical impedance spectra reveal that the reconstructed cathode/electrolyte interface promotes the kinetics of active cations and induces the less potential‐dependent charge storage process. Consequently, TiO2 exhibits a remarkable rate performance (discharge capacity of 68.9 mAh g−1 at 1 A g−1) and long‐lifespan over 3000 cycles at 0.5 A g−1. [ABSTRACT FROM AUTHOR]

Aqueous zinc‐iodine (Zn‐I2) batteries are promising candidates for grid‐scale energy storage due to their safety and cost‐effectiveness. However, the shuttle effect of polyiodides, Zn corrosion, and accumulation of by‐products restrict their applications. Herein, a simple vermiculite nanosheets (VS) suspension electrolyte is designed for simultaneous confinement of polyiodides and stabilization of Zn anode. It is found that the generation of I5− as dominant intermediate and the precipitation reaction between I5− and alkaline by‐products should cause irreversible iodine species loss. Benefiting from the high binding energy between polyiodides and silica‐oxygen bonds of VS, dissolved polyiodides are effectively anchored on the surface of VS suspended in the bulk electrolyte to suppress the shuttle effect, which is confirmed by in situ Raman, Ultraviolet‐visible characterizations and theoretical calculations. Furthermore, the self‐assembly VS interfacial layer on the surface of Zn anode hinders side reactions induced by polyiodides. Meanwhile, the interlayer and surface excess negative charges of VS tend to be compensated by Zn2+ from diffuse layer, which serves as ion accelerators for transferring Zn2+ at the interface immediately, rendering dendrite‐free Zn plating/stripping behavior. Consequently, the Zn‐I2 battery with VS electrolyte achieves an ultra‐long lifespan of 40000 cycles with a negligible capacity decay at 20 C. [ABSTRACT FROM AUTHOR]

Zn−I2 batteries stand out in the family of aqueous Zn‐metal batteries (AZMBs) due to their low‐cost and immanent safety. However, Zn dendrite growth, polyiodide shuttle effect and sluggish I2 redox kinetics result in dramatically capacity decay of Zn−I2 batteries. Herein, a Janus separator composed of functional layers on anode/cathode sides is designed to resolve these issues simultaneously. The cathode layer of Fe nanoparticles‐decorated single‐wall carbon nanotubes can effectively anchor polyiodide and catalyze the redox kinetics of iodine species, while the anode layer of cation exchange resin rich in −SO3− groups is beneficial to attract Zn2+ ions and repel detrimental SO42−/polyiodide, improving the stability of cathode/anode interfaces synergistically. Consequently, the Janus separator endows outstanding cycling stability of symmetrical cells and high‐areal‐capacity Zn−I2 batteries with a lifespan over 2500 h and a high‐areal capacity of 3.6 mAh cm−2. [ABSTRACT FROM AUTHOR]

Zn−I2 batteries stand out in the family of aqueous Zn‐metal batteries (AZMBs) due to their low‐cost and immanent safety. However, Zn dendrite growth, polyiodide shuttle effect and sluggish I2 redox kinetics result in dramatically capacity decay of Zn−I2 batteries. Herein, a Janus separator composed of functional layers on anode/cathode sides is designed to resolve these issues simultaneously. The cathode layer of Fe nanoparticles‐decorated single‐wall carbon nanotubes can effectively anchor polyiodide and catalyze the redox kinetics of iodine species, while the anode layer of cation exchange resin rich in −SO3− groups is beneficial to attract Zn2+ ions and repel detrimental SO42−/polyiodide, improving the stability of cathode/anode interfaces synergistically. Consequently, the Janus separator endows outstanding cycling stability of symmetrical cells and high‐areal‐capacity Zn−I2 batteries with a lifespan over 2500 h and a high‐areal capacity of 3.6 mAh cm−2. [ABSTRACT FROM AUTHOR]

Based on the in-depth understanding of Li0 deposition behavior, a high interfacial-energy artificial SEI with rich LiF embedded in PAMPS-Li polymer network is designed to realize favorable Li0 nucleation and rapid desolvation of Li+ simultaneously, reveals the importance of interfacial energy for highly reversible Li0 deposition/stripping. [Display omitted] High interfacial energy Li0-electrolyte interface contributes to larger Li0 nucleation embryos and a more stable interface, so the interfacial energy is essential for highly reversible Li0 deposition/stripping. Herein, a high interfacial-energy artificial solid electrolyte interphase (SEI) with rich LiF embedded in lithiated poly-2-acrylamido-2-methylpropane sulfonic acid (PAMPS-Li) network is designed to realize favorable Li0 nucleation and rapid desolvation of Li+ simultaneously. The Li−F bonds in LiF (0 0 1) exhibit stronger ion–dipole interactions with Li atoms, offering higher interfacial energies. When the growth surface energy and total interfacial energy of Li0 are balanced, the high interfacial energy SEI with abundant LiF can promote the formation of larger Li0 nucleation embryos. In addition, the PAMPS-Li with immobilized anions presents weaker interaction with Li0 and possesses higher polymer-Li interfacial energy, and its amide and sulfonic acid groups exhibit higher binding energies with Li+. Therefore, PAMPS-Li can easily promote the Li+ to escape from the solvent sheath and weaken the desolvation energy barrier. The highly reversible Li0 deposition behavior with restricted side reactions is achieved based on the synergistic modification of high interfacial energy SEI with heterostructure. Most importantly, lifespan of multi-layered Li0 pouch cell (330 Wh kg−1) with a low N/P ratio (1.67) is over 100 cycles, verifying its potential practical application. [ABSTRACT FROM AUTHOR]

For zinc‐metal batteries, the instable chemistry at Zn/electrolyte interphasial region results in severe hydrogen evolution reaction (HER) and dendrite growth, significantly impairing Zn anode reversibility. Moreover, an often‐overlooked aspect is this instability can be further exacerbated by the interaction with dissolved cathode species in full batteries. Here, inspired by sustained‐release drug technology, an indium‐chelated resin protective layer (Chelex‐In), incorporating a sustained‐release mechanism for indium, is developed on Zn surface, stabilizing the anode/electrolyte interphase to ensure reversible Zn plating/stripping performance throughout the entire lifespan of Zn//V2O5 batteries. The sustained‐release indium onto Zn electrode promotes a persistent anticatalytic effect against HER and fosters uniform heterogeneous Zn nucleation. Meanwhile, on the electrolyte side, the residual resin matrix with immobilized iminodiacetates anions can also repel detrimental anions (SO42− and polyoxovanadate ions dissolved from V2O5 cathode) outside the electric double layer. This dual synergetic regulation on both electrode and electrolyte sides culminates a more stable interphasial environment, effectively enhancing Zn anode reversibility in practical high‐areal‐capacity full battery systems. Consequently, the bio‐inspired Chelex‐In protective layer enables an ultralong lifespan of Zn anode over 2800 h, which is also successfully demonstrated in ultrahigh areal capacity Zn//V2O5 full batteries (4.79 mAh cm−2). [ABSTRACT FROM AUTHOR]

For zinc‐metal batteries, the instable chemistry at Zn/electrolyte interphasial region results in severe hydrogen evolution reaction (HER) and dendrite growth, significantly impairing Zn anode reversibility. Moreover, an often‐overlooked aspect is this instability can be further exacerbated by the interaction with dissolved cathode species in full batteries. Here, inspired by sustained‐release drug technology, an indium‐chelated resin protective layer (Chelex‐In), incorporating a sustained‐release mechanism for indium, is developed on Zn surface, stabilizing the anode/electrolyte interphase to ensure reversible Zn plating/stripping performance throughout the entire lifespan of Zn//V2O5 batteries. The sustained‐release indium onto Zn electrode promotes a persistent anticatalytic effect against HER and fosters uniform heterogeneous Zn nucleation. Meanwhile, on the electrolyte side, the residual resin matrix with immobilized iminodiacetates anions can also repel detrimental anions (SO42− and polyoxovanadate ions dissolved from V2O5 cathode) outside the electric double layer. This dual synergetic regulation on both electrode and electrolyte sides culminates a more stable interphasial environment, effectively enhancing Zn anode reversibility in practical high‐areal‐capacity full battery systems. Consequently, the bio‐inspired Chelex‐In protective layer enables an ultralong lifespan of Zn anode over 2800 h, which is also successfully demonstrated in ultrahigh areal capacity Zn//V2O5 full batteries (4.79 mAh cm−2). [ABSTRACT FROM AUTHOR]

Porous Graphitic carbon nitride(pg‐C3N4) possessing hierarchical pores and lamellar nanostrucutres was synthesized in the absent of templates by pyrolysis of the solution‐assisted mixing dual‐precursors. The samples were characterized by X‐ray diffraction, scanning electron microscopy, transmission electron microscopy, N2 porosimeter, X‐ray photoelectron spectroscopy, UV‐Vis andphotoluminescence spectroscopy.The photocatalytic activities of as‐prepared materials for degradation of methyl violet were studied. The results show that the as‐prepared g‐C3N4consists of well‐dispersed layers with uniform sizeand hierarchical (Meso/Macro) pores in the nanosheets, which favor photogenerated electron‐hole pairs'separation, and the degradation of methyl violet conforms to the quasi‐first‐order kinetic model. The porous g‐C3N4 synthesized by optimizing precursors' ratios exhibited faster degradation rate than g‐CN material in the process of photocatalyzing methyl violet andthe degradation rate was over 93 % after irradiation of 180 min, implying that the as‐prepared hierarchically porous g‐C3N4 is a high‐effective and metal‐free photocatalytic material for degradation of pollutants. [ABSTRACT FROM AUTHOR]

A dual-salt ether-based localized high-concentration electrolyte is designed to generate salt-derived interfacial layers, enabling high-voltage lithium metal batteries to operate in a wide-temperature range from −40 °C to 80 °C. The diluent is demonstrated to effectively improve the reversibility of lithium and oxidation stability of the electrolyte due to its modification of SEI formation and low HOMO energy level. [Display omitted] • Dual-salt LHCE promotes the formation of salt-derived interfacial layers. • The presence of diluent TTE enables mild and controllable SEI formation. • The average Coulombic efficiency of Li||Cu cells is 99.5 % at 0.5 mA cm−2. • Stable cycling of 4.5 V-Li||NCM523 full-cell (N/P ≈ 0.9) is achieved. • The electrolyte exhibits excellent wide temperature performance. Wide-temperature and high-voltage lithium metal batteries (LMBs) have great potential in electric vehicles, but their applications face major challenges due to unstable interfacial layers. Here, a dual-salt (lithium bis(trifluoromethanesulfonyl) and lithium difluoro(oxalato)borate) ether-based localized high-concentration electrolyte (LHCE) is designed to facilitate the formation of salt-derived interfacial layers. It is proved that the presence of diluent makes the formation of solid electrolyte interphase (SEI) mild and controllable, thereby avoiding the overproduction of reduction product and improving the reversibility of lithium metal anode. Therefore, the electrolyte achieves a high average Coulombic efficiency (CE) of 99.5 % for Li||Cu cell and stable cycling of 4.5 V Li||LiNi 0.5 Co 0.2 Mn 0.3 O 2 (NCM523) cell. Benefiting from the excellent compatibility of electrolyte with electrodes, the Li||NCM523 full-cell provides excellent cycling stability under severe conditions (4.5 V, negative/positive capacity ratio ≈ 0.9). Furthermore, the electrolyte exhibits excellent wide-temperature electrochemical performance, enabling the cells to provide 71 % of room-temperature capacity at −40 °C and retain 85 % capacity retention after 200 cycles with high CE at 80 °C. This study shares a new insight into the role of diluent and provides a promising strategy for electrolyte design of wide-temperature and high-voltage LMBs. [ABSTRACT FROM AUTHOR]