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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]

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]