Search

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]

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]

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]

The emerging rocking-chair aqueous zinc-ion battery (AZIB) configuration provides a promising approach for realizing their practical applications by avoiding the critical drawbacks of Zn metal anodes including unsatisfactory Coulombic efficiency and low Zn utilization. Therefore, exploiting appropriate insertion-type anodes with fast charge-transfer kinetics is of great importance, and many modifications focusing on the improvement of electron transport and bulk Zn2+ diffusion have been proposed. However, the interfacial Zn2+ transfer determined by the desolvation process actually dominates the kinetics of overall battery reactions, which is mainly overlooked. Herein, the interlayer structure of MoS2 is rationally co-intercalated with water and ethylene glycol (EG) molecules (MoS2@EG), giving rise to a fast non-desolvation Zn2+ storage mechanism, which is verified by the extraordinarily smaller activation energy of interfacial Zn2+ transfer (4.66 kJ mol−1) compared with that of pristine MoS2 (56.78 kJ mol−1). Furthermore, the results of theoretical calculations, in-situ Raman and ex-situ characterizations also indicate the enhanced structural integrity of MoS2@EG during cycling due to the enlarged interlayer spacing and charge screening effect induced by interlaminar EG molecules. Consequently, the MoS2@EG anode enables excellent cycling stability of both high-energy-density MoS2@EG∥PVO (polyaniline intercalated V2O5) and high-voltage MoS2@EG∥Na3V2(PO4)2O2F (NVPF) full batteries with neglectable capacity decay at −20 °C. [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]

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//V 2 O 5 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 (SO 4 2- and polyoxovanadate ions dissolved from V 2 O 5 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//V 2 O 5 full batteries (4.79 mAh cm -2 )., (© 2024 Wiley-VCH GmbH.)

Zn-I 2 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 I 2 redox kinetics result in dramatically capacity decay of Zn-I 2 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 -SO 3 - groups is beneficial to attract Zn 2+ ions and repel detrimental SO 4 2- /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-I 2 batteries with a lifespan over 2500 h and a high-areal capacity of 3.6 mAh cm -2 ., (© 2023 Wiley-VCH GmbH.)