Regulating the Zn deposition orientation is an efficient way to suppress Zn dendrites and stabilize Zn anodes in aqueous Zn ion batteries (ZIBs). Few studies have been conducted to control Zn(002) deposition by altering the Zn2+ solvation structure with a cosolvent. Herein, the bifunctional high-polarity cosolvent hexamethylphosphoramide (HMPA) is proposed in an aqueous electrolyte. It not only suppresses the H2 evolution reaction via the reshaped Zn2+ solvation structure with decreased H2O activity but also induces Zn(002) deposition with a hexagonal-close-packed morphology due to the strong absorption ability of HMPA to Zn(002). With the optimized electrolyte, Zn dendrites and the HER are suppressed and an ultralong cycle life of 1500 cycles with 99.6% Coulombic efficiency is achieved in Zn||Cu cells. Zn||NH4V5O10 and Zn||polyaniline full cells exhibit improved cycling performances compared to that of the bare electrolyte. Our finding provides a feasible and promising way to stabilize Zn anodes and promote the commercial application of ZIBs. 

Regulating Zn(002) Deposition toward Long Cycle Life for Zn Metal Batteries

Advanced aqueous batteries are promising for next generation flexible and wearable devices owing to the high safety, yet still requiring better cycling stability and high specific capacity in wide temperature range. Herein, a polymeric acid hydrogel electrolyte (PAGE) with 3 M Zn(ClO4)2 was fabricated for high performance Zn/polyaniline (PANI) batteries. The -SO3-H+ function group in PAGE can endow the Zn/PANI battery with following merits: firstly, accelerating the redox reaction kinetics for PANI by constant proton generation; secondly, increasing the specific capacity by boosting the reaction sites between ions and PANI functional groups; thirdly, suppressing the side reaction and dendrites by inducing the (002) crystal plane formation. In addition, the anti-freezing performance for the hydrogel is also optimized by the salt and hydrogel, with a high ionic conductivity of 14.2 mS cm-1 at -35oC. As a consequence, even at -35oC, the Zn/Zn symmetrical battery can keep stable for more than 1,500 h under 2 mA cm-2, and the Zn/PANI battery can provide ultra-high stable specific capacity of 79.6 mA h g-1 for more than 70,000 cycles at 15 A g-1. This proton-supplying strategy by polymeric acid hydrogel may further propel the development of high performance aqueous batteries.

Proton-reservoir hydrogel electrolyte for long-term cycling Zn/PANI batteries in wide temperature range.

In situ formation of a stable interphase layer on zinc surface is an effective solution to suppress dendrite growth. However, the fast transport of bivalent Zn-ions within the solid interlayer remains very challenging. Herein, we engineer the SEI components and enable superior kinetics of Zn metal batteries under harsh conditions through regulating the sequence of interfacial chemical reaction. With the differences in chemical reactivity of trimethyl phosphate co-solvent and trifluoromethanesulfonate anions in the Zn2+-solvation shell, Zn3(PO4)2 and ZnF2 are successively generated on Zn metal surface to form a gradient ZnF2-Zn3(PO4)2 interphase. Mechanistic studies reveal the outer ZnF2 facilitates Zn2+ desolvation and inner Zn3(PO4)2 serves as channels for fast Zn2+ transport, contributing to long-term cycling at subzero temperatures. Impressively, the gradient SEI enables a high lifespan over 7000 hours in Zn symmetric cell and a capacity retention of 86.1% after 12000 cycles in Zn-KVOH full cell at -50 °C. 

Regulating interfacial reaction through electrolyte chemistry enables gradient interphase for low-temperature zinc metal batteries.

Carbonate electrolytes have excellent chemical stability and high salt solubility, which is ideally practical choice for achieving high energy density sodium (Na) metal battery at room temperature. However, their application at ultra-low temperature (-40 oC) is adversely affected by the instability of solid electrolyte interphase (SEI) formed by electrolyte decomposition and the difficulty of desolvation. Here, we designed a novel low-temperature carbonate electrolyte by molecular engineering on solvation structure. The calculations show that ethylene sulfate (ES) inhibits solvent decomposition and reduces the sodium ion desolvation energy. In addition, experimental results demonstrate that ES promotes the forming of more inorganic substances on the Na surface, which inhibits dendrite growth and increases ionic conductivity. At -40 oC, the Na||Na symmetric battery exhibits a stable cycle of 1500 hours, and the Na||Na3V2(PO4)3 (NVP) battery achieves 88.2% capacity retention after 200 cycles. Our work provides a new way to develop high energy density sodium metal battery under extreme low temperature environment.

Molecular Engineering on Solvation Structure of Carbonate Electrolyte toward Durable Sodium Metal Battery at -40 oC.

Constructing an inorganic-rich and robust solid electrolyte interphase (SEI) is one of the crucial approaches to improving the electrochemical performance of sodium metal batteries (SMBs). However, the low conductivity and distribution of common inorganics in SEI disturb Na+ diffusion and induce nonuniform sodium deposition. Here, we construct a unique SEI with evenly scattered high-conductivity inorganics by introducing a self-sacrifice LiTFSI into the sodium salt-base carbonate electrolyte. The reductive competition effect between LiTFSI and FEC facilitates the formation of the SEI with evenly scattered inorganics. In which the high-conductive Li3N and inorganics provide fast ions transport domains and high-flux nucleation sites for Na+, thus conducive to rapid sodium deposition at a high rate. Therefore, the SEI derived from LiTFSI and FEC enables the Na∥Na3V2(PO4)3 cell to show 89.15% capacity retention (87.62 mA h g-1) at an ultrahigh rate of 60 C after 10,000 cycles, while the cell without LiTFSI delivers only 48.44% capacity retention even after 8000 cycles. Moreover, the Na∥Na3V2(PO4)3 pouch cell with the special SEI presents a stable capacity retention of 92.05% at 10 C after 2000 cycles. This unique SEI design elucidates a new strategy to propel SMBs to operate under extreme high-rate conditions.

Reductive Competition Effect-Derived Solid Electrolyte Interphase with Evenly Scattered Inorganics Enabling Ultrahigh Rate and Long-Life Span Sodium Metal Batteries.

Low-temperature and high-rate sodium metal batteries enabled by electrolyte chemistry

π-π stacking controlled photochromic/thermochromic properties of salicylaldehyde Schiff base in solid state

A Comprehensive Experiment of Synthesis and Photochromic Characterization of Rhodamine 6G Hydrazide Salicylaldehyde Schiff Base Zinc Ion Complex

Highly Reversible and Stable Zn Metal Anode under Wide Temperature Conditions Enabled by Modulating Electrolyte Chemistry

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Low-temperature and high-rate sodium metal batteries enabled by electrolyte chemistry

π-π stacking controlled photochromic/thermochromic properties of salicylaldehyde Schiff base in solid state

A Comprehensive Experiment of Synthesis and Photochromic Characterization of Rhodamine 6G Hydrazide Salicylaldehyde Schiff Base Zinc Ion Complex

Highly Reversible and Stable Zn Metal Anode under Wide Temperature Conditions Enabled by Modulating Electrolyte Chemistry