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The corrosion, parasitic reactions, and aggravated dendrite growth severely restrict development of aqueous Zn metal batteries. Here, we report a novel strategy to break the hydrogen bond network between water molecules and construct the Zn(TFSI)2‐sulfolane‐H2O deep eutectic solvents. This strategy cuts off the transfer of protons/hydroxides and inhibits the activity of H2O, as reflected in a much lower freezing point (<−80 °C), a significantly larger electrochemical stable window (>3 V), and suppressed evaporative water from electrolytes. Stable Zn plating/stripping for over 9600 h was obtained. Based on experimental characterizations and theoretical simulations, it has been proved that sulfolane can effectively regulate solvation shell and simultaneously build the multifunctional Zn‐electrolyte interface. Moreover, the multi‐layer homemade modular cell and 1.32 Ah pouch cell further confirm its prospect for practical application. [ABSTRACT FROM AUTHOR]

Rechargeable aqueous Zn‐ion batteries (ZIBs) are always regarded as a promising energy storage device owing to their higher safety and durability. However, two problems have become the main trouble for the practical application of ZIBs such as the dendrite growth of Zn metal anode in electrolyte and the freezing of water solvent at low temperature. Herein, to overcome these challenges, a new strategy, multi‐component crosslinked hydrogel electrolyte, is proposed to inhibit Zn dendrites and realize low temperature environmental adaptability for ZIBs. Benefitting from the superior inhibition effect of the polyacrylamide and dimethyl sulfoxide (DMSO) on Zn dendrites, the coulombic efficiency of the symmetric cell of ≈99.5% is achieved during the Zn plating/stripping over 1 300 h, and the assembled full‐cell demonstrates the large specific capacity of 265.2 mAh g‐1 and high cyclic stability with the capacity retention of 95.27% after 3 000 cycles. In addition, the full‐cell delivers stable operation at a wide temperature range, from 60 to −40 °C, due to the introduction of additive DMSO. This work provides an inspired strategy and novel opportunities to realize a dendrite‐free and wide‐temperature rechargeable aqueous Zn‐ion energy storage system. [ABSTRACT FROM AUTHOR]

Rechargeable aqueous zinc ion batteries have attracted increasing attention as a new energy storage system because of the high ionic conductivity and safe aqueous electrolyte. The spontaneous vanadium dissolution in aqueous electrolytes is one major problem because the water with serious polarity would corrode the crystal structure of vanadium‐based cathodes. Here, an in situ artificial cathode electrolyte interphase (CEI) strategy is proposed to kinetically suppress the vanadium dissolution in aqueous zinc ion batteries. The strontium ion is introduced into vanadium oxide layers as a sacrifice guest, which would directly precipitate upon getting out from the vanadium‐based cathode to in situ from a CEI coating layer on the surface. This strategy is proven with the help of various technologies, and the remarkable ability of the CEI layer to suppress cathode dissolution is evaluated by multiple electrochemical and chemical methods. As a result, the cathode after CEI conversion exhibits the best recharge capacity retention after open circuit voltage rest for 3 days in comparison with other cathodes. This work reports a general strategy to construct the electrode‐electrolyte interface for suppressing vanadium‐based cathodes dissolution in aqueous electrolytes and beyond. [ABSTRACT FROM AUTHOR]

Two dimensional (2D) heterojunction based on g‐C3N4 and CuInS2(CIS) nanosheets has been successfully constructed with the assistance of biomolecules L‐cysteine. We demonstrated that a typical p–n junction charges transfer mode of CIS/PCN (protonated g‐C3N4) can be switched to Z‐scheme transfer mode through the integration of Au by weakening the role of built‐in electric field. The morphology of CIS/Au/PCN can be well adjusted through the formation of Au−S covalent bond and the electrostatic adsorption between Au and PCN during the hydrothermal process. Furthermore, the intimate interface contact inside CIS/Au/PCN heterojunction was indeed constructed, which may promote the charges separation and transfer process at the interface as evidenced by ESR spectra and time‐resolved PL spectra. Under visible light illumination, the CIS/Au/PCN exhibited an enhanced CO (19.46 μmol/g) and CH4 (1.18 μmol/g) yield in CO2 reduction, which was about 5.04 times and 2.03 times higher than pure PCN. The composite heterojunction also showed excellent photocatalytic activity for tetracycline degradation with a 87 % degradation efficiency in 1 hour, which was 2.07 times higher than pure PCN. The experimental and theoretical calculation results demonstrated that an all‐solid‐state Z‐scheme heterojunction was formed in the CIS/Au/PCN system, which was different from the typical p–n junction charges transfer mechanism in CIS/PCN. [ABSTRACT FROM AUTHOR]

Maximizing the activity of materials towards the alkaline hydrogen evolution reaction while maintaining their structural stability under realistic working conditions remains an area of active research. Herein, we report the first controllable surface modification of graphene(G)/V8C7 heterostructures by nitrogen. Because the introduced N atoms couple electronically with V atoms, the V sites can reduce the energy barrier for water adsorption and dissociation. Investigation of the multi‐regional synergistic catalysis on N‐modified G/V8C7 by experimental observations and density‐functional‐theory calculations reveals that the increase of electron density on the epitaxial graphene enable it to become favorable for H* adsorption and the subsequent reaction with another H2O molecule. This work extends the range of surface‐engineering approaches to optimize the intrinsic properties of materials and could be generalized to the surface modification of other transition‐metal carbides. [ABSTRACT FROM AUTHOR]