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.

Although Mn2+ additive alleviates the dissolution issue of Mn-based cathodes in aqueous zinc-ion batteries (ZIBs), problems including complex side reactions and abnormal capacity fluctuation pose new challenges for their large-scale...

Sulfur-based aqueous zinc batteries (SZBs) attract increasing interest due to their integrated high capacity, competitive energy density, and low cost. However, the hardly reported anodic polarization seriously deteriorates the lifespan and energy density of SZBs at a high current density. Here, we develop an integrated acid-assisted confined self-assembly method (ACSA) to elaborate a two-dimensional (2D) mesoporous zincophilic sieve (2DZS) as the kinetic interface. The as-prepared 2DZS interface presents a unique 2D nanosheet morphology with abundant zincophilic sites, hydrophobic properties, and small-sized mesopores. Therefore, the 2DZS interface plays a bifunctional role in reducing the nucleation and plateau overpotential: (a) accelerating the Zn 2+ diffusion kinetics through the opened zincophilic channels and (b) inhibiting the kinetic competition of hydrogen evolution and dendrite growth via the significant solvation−sheath sieving effect. Therefore, the anodic polarization is reduced to 48 mV at 20 mA cm −2 , and the full-battery polarization is reduced to 42% of an unmodified SZB. As a result, an ultrahigh energy density of 866 Wh kg sulfur −1 at 1 A g −1 and a long lifespan of 10,000 cycles at a high rate of 8 A g −1 are achieved.