Molybdenum Sulfide Nanoflowers as Electrodes for Efficient and Scalable Lithium-Ion Capacitors.

Hybrid supercapacitors (HSCs) bridge the unique advantages of batteries and capacitors and are considered promising energy storage devices for hybrid vehicles and other electronic gadgets. Lithium-ion capacitors (LICs) have attained particular interest due to their higher energy and power density than traditional supercapacitor devices. The limited voltage window and the deterioration of anode materials upsurged the demand for efficient and stable electrode materials. Two-dimensional (2D) molybdenum sulfide (MoS2) is a promising candidate for developing efficient and durable LICs due to its wide lithiation potential and unique layer structure, enhancing charge storage efficiency. Modifying the extrinsic features, such as the dimensions and shape at the nanoscale, serves as a potential path to overcome the sluggish kinetics observed in the LICs. Herein, the MoS2 nanoflowers have been synthesized through a hydrothermal route. The developed LIC exhibited a specific capacitance of 202.4 F g­1 at 0.25 A g­1 and capacitance retention of > 90% over 5,000 cycles. Using an ether electrolyte improved the voltage window (2.0 V) and enhanced the stability performance. The ex-situ material characterization after the stability test reveals that the storage mechanism in MoS2-LICs is not diffusion-controlled. Instead,  fast surface redox reactions, especially intercalation/deintercalation, are more prominent for charge storage.

Unveiling the Mysteries: Acetonitrile's Dance with Weakly-Solvating Electrolytes in Shaping Gas Evolution and Electrochemical Performance of Zinc-ion Batteries.

Aqueous Zn-metal battery (AZMB) is a promising candidate for future large-scale energy storage with commendable capacity, exceptional safety characteristics, and low cost. Acetonitrile (AN) has been widely used as an effective electrolyte constituent to improve AZMBs' performance. However, its functioning mechanisms remain unclear. In this study, we unveiled the critical roles of AN in AZMBs via comparative in situ electrochemical, gaseous, and morphological analyses. Despite its limited ability to solvate Zn ions, AN-modulated Zn-ion solvation sheath with increased anions and decreased water achieves a weakly-solvating electrolyte. As a result, the Zn||Zn cell with AN addition exhibited 63 times longer cycle life than cell without AN and achieved a 4 Ah cm-2 accumulated capacity with no H2 generation. In V2O5||Zn cells, for the first time, AN suppressing CO2 generation, elevating CO2-initiation voltage from 2→2.44 V (H2: 2.43→2.55 V) was discovered. AN-impeded transit and Zn-side deposition of dissolved vanadium ions, known as "crosstalk," ameliorated inhomogeneous Zn deposition and dendritic Zn growth. At last, we demonstrated an AN-enabled high-areal-capacity AZMB (3.3 mAh cm-2) using high-mass-loading V2O5 cathode (26 mg cm-2). This study shed light on the strategy of constructing fast-desolvation electrolytes and offered insights for future electrolyte accommodation for high-voltage AZMB cathodes.

Regulating Zinc Nucleation Sites and Electric Field Distribution to Achieve High-Performance Zinc Metal Anode via Surface Texturing.

Understanding zinc (Zn) deposition behavior and improving Zn stripping and plating reversibility are significant in developing practical aqueous Zn ion batteries (AZIBs). Zn metal is abundant, cost-effective, and intrinsically safe compared with Li. However, their similar inhomogeneous growth regime harms their practicality. This work reports a facile, easily scalable, but effective method to develop a textured Zn with unidirectional scratches on the surface that electrochemically achieves a high accumulated areal capacity of 5530 mAh cm-2 with homogenized Zn deposition. In symmetric cells, textured Zn presents a stable cycling performance of 1100 hours (vs 250 h of bare Zn) at 0.5 mA cm-2 for 0.5 mAh cm-2 and lower nucleation and plating overpotentials of 120.5 and 41.8 mV. In situ optical microscopy and COMSOL simulation disclose that the textured surface topography can 1) homogenize the electron field distribution on the Zn surface and regulate Zn nucleation and growth, and 2) provides physical space to accommodate Zn deposits, prevent the detachment of "dead" Zn, and improve the structural sufficiency of Zn anode. Moreover, differential electrochemical mass spectrometry analysis find that the textured Zn with regulated interfacial electron activity also presents a higher resistance toward hydrogen evolution and other parasitic reactions.

Eutectic Electrolytes Chemistry for Rechargeable Zn Batteries.

Rechargeable zinc batteries (RZBs) have proved to be promising candidates as an alternative to lithium-ion batteries due to their low cost, inherent safety, and environmentally benign features. While designing cost-effective electrolyte systems with excellent compatibility with electrode materials, high energy/power density as well as long life-span challenge their further application as grid-scale energy storage devices. Eutectic electrolytes as a novel class of electrolytes have been extensively reported and explored taking advantage of their feasible preparation and high tunability. Recently, some perspectives have summarized the development and application of eutectic electrolytes in metal-based batteries, but their infancy requires further attention and discussion. This review systematically presents the fundamentals and definitions of eutectic electrolytes. Besides, a specific classification of eutectic electrolytes and their recent progress and performance on RZB fields are introduced as well. Significantly, the impacts of various composing eutectic systems are disserted for critical RZB chemistries including attractive features at electrolyte/electrode interfaces and ions/charges transport kinetics. The remaining challenges and proposed perspectives are ultimately induced, which deliver opportunities and offer practical guidance for the novel design of advanced eutectic electrolytes for superior RZB scenarios.