While research interest in aqueous batteries has surged due to their intrinsic low cost and high safety, the practical application is plagued by the restrictive capacity (less than 600 mAh g −1 ) of electrode materials. Sulfur-based aqueous batteries (SABs) feature high theoretical capacity (1672 mAh g −1 ), compatible potential, and affordable cost, arousing ever-increasing attention and intense efforts. Nonetheless, the underlying electrochemistry of SABs remains unclear, including complicated thermodynamic evolution and insufficient kinetics metrics. Consequently, multifarious irreversible reactions in various application systems imply the systematic complexity of SABs. Herein, rather than simply compiling recent progress, this Perspective aims to construct a theory-to-application methodology. Theoretically, attention has been paid to a critical appraisal of the aqueous-S-related electrochemistry, including fundamental properties evaluation, kinetics metrics with transient and steady-state analyses, and thermodynamic equilibrium and evolution. To put it into practice, current challenges and promising strategies are synergistically proposed. Practically, the above efforts are employed to evaluate and develop the device-scale applications, scilicet flow-SABs, oxide-SABs, and metal-SABs. Last, chemical and engineering insights are rendered collectively for the future development of high-energy SABs.
Poor thermodynamic stability and sluggish electrochemical kinetics of metallic Zn anode in aqueous solution greatly hamper its practical application. To solve such problems, to date, various zincophilic surface modification strategies are developed, which can facilitate reversible Zn plating/stripping behavior. However, there is still a lack of systematic and fundamental understanding regarding the metrics of thermodynamics inertia and kinetics zincophilia in selecting zincophilic sites. Herein, hetero‐metallic interfaces are prioritized for the first time via optimizing different hetero metals (Fe, Co, Ni, Sn, Bi, Cu, Zn, etc.) and synthetic solvents (ethanol, ethylene glycol, n‐propanol, etc.). Specifically, both theoretical simulations and experimental results suggest that this Bi@Zn interface can exhibit high efficiency owing to the thermodynamics inertia and kinetics zincophilia. A best practice for prioritizing zincophilic sites in a more practical metric is also proposed. As a proof of concept, the Bi@Zn anode delivers ultralow overpotential of ≈55 mV at a high rate of 10 mA cm−2 and stable cycle life over 4700 cycles. The elaborated “thermodynamics inertia and kinetics metalphilia” metrics for hetero‐metallic interfaces can benchmark the success of other metal‐based batteries.
Sulfur-based aqueous batteries (SABs) are deemed promising candidates for safe, low-cost, and high-capacity energy storage. However, despite their high theoretical capacity, achieving high reversible value remains a great challenge due to the thermodynamic and kinetics problems of elemental sulfur. Here, the reversible six-electron redox electrochemistry is constructed by activating sulfur oxidation reaction (SOR) process of the elaborate mesocrystal NiS2 (M-NiS2). Through the unique 6e− solid-to-solid conversion mechanism, the SOR efficiency can reach an unprecedented degree of ca. 96.0%. The SOR efficiency is further revealed to be closely associated with the kinetics feasibility and thermodynamic stability of the M-NiS2 intermedium in the formation of elemental sulfur. Benefiting from the boosted SOR, compared with the bulk electrode, the M-NiS2 electrode exhibits a high reversible capacity (1258 mAh g−1), ultrafast reaction kinetics (932 mAh g−1 at 12 A g−1), and long-term cyclability (2000 cycles at 20 A g−1). As a proof of concept, a new M-NiS2||Zn hybrid aqueous battery exhibits an output voltage of 1.60 V and an energy density of 722.4 Wh kgcath−1, which opens a new opportunity for the development of high-energy aqueous batteries.
With the popularization of wide band-gap power modules in offshore wind power systems and water surface photovoltaic power stations, packaging materials face challenges of corrosion by salt, blended with high humidity. Copper-silver (Cu-Ag) composite sintered paste was proposed by researchers as a novel die-attach material for a lower cost and antielectromigration ability. However, the potential difference between copper and silver forms galvanic corrosion in a highhumidity environment, resulting in accelerated failure combined with salt mist. To further promote the application of composite sintered materials, a copper-silver double-sphere galvanic corrosion model based on finite element simulation was proposed in this paper. The relationship between corrosion rate and time of different Cu-Ag particle size combinations under different sintering degrees was predicted by initial exchange current density. Through the electrochemical characterization of the sintered samples, the optimal combination of materials was further discussed. The accuracy of the model was also verified. The conclusions obtained from both the experiments and simulation work provide guidance for future anti-corrosion analysis, as well as the reliability improvement of novel composite sintered materials.
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