2D Mesoporous Zincophilic Sieve for High-Rate Sulfur-Based Aqueous Zinc Batteries

Abstract

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.

Minireview on Aqueous Zinc–Sulfur Batteries: Recent Advances and Future Perspectives

“…It maintains a stable performance for over 300 cycles at a rate of 2 C, experiencing minimal capacity degradation with a fading rate of approximately 0.17% per cycle. In an effort to reduce anodic polarization in an AZSB, Liu et al devolped a two-dimensional (2D) mesoporous zincophilic sieve (2DZS) as a kinetic interface. The 2DZS showcases a unique nanosheet structure and hydrophobic characteristics, characterized by a high density of zincophilic sites and small-sized mesopores..…”

“…(c) GCD curve of an OS||Zn@2DZS battery at 1 A g –1 . This panel was reproduced from ref . Copyright 2023 American Chemical Society.…”

Polycation‐Regulated Electrolyte and Interfacial Electric Fields for Stable Zinc Metal Batteries

“…Dramatic progress has been accomplished in the pursuit of high performance cathode materials such as transition metal (manganese, vanadium) oxide, organic molecule, and so on [1–5] . Nevertheless, unbounded dendrite growth, corrosion and passivation of zinc (Zn) metal anodes, resulting in low coulombic efficiency (CE) and limited lifetime, which may lead to battery short circuit, is one of the most crucial obstacles for the development of aqueous ZIBs [6–12] . Several strategies have been executed to enhance the electrochemical stability of Zn metal anodes by inhibiting the dendrite formation and banishing the water‐induced parasitic reaction, including electrolyte regulation, interfacial manipulation, substrate modification, etc [13–26] .…”

“…[1][2][3][4][5] Nevertheless, unbounded dendrite growth, corrosion and passivation of zinc (Zn) metal anodes, resulting in low coulombic efficiency (CE) and limited lifetime, which may lead to battery short circuit, is one of the most crucial obstacles for the development of aqueous ZIBs. [6][7][8][9][10][11][12] Several strategies have been executed to enhance the electrochemical stability of Zn metal anodes by inhibiting the dendrite formation and banishing the water-induced parasitic reaction, including electrolyte regulation, interfacial manipulation, substrate modification, etc. [13][14][15][16][17][18][19][20][21][22][23][24][25][26] Among these strategies, electrolyte formulation plays a vital role in regulating the Zn deposition behavior and diminishing the side reaction on Zn metal anodes, because of its effectiveness, simple procedure, and easy implementation.…”

A mesoporous Al2O3 zincophilic sieve enables ultra-long lifespan of Zn-ion batteries

“…When the electrolyte enters different pore sizes of the mesoporous sieve, the solvation structure in a limited space can be changed. 19 According to the Eigen-Tamm mechanism, 11 when ZnSO 4 dissolves in water, most of the Zn 2+ (CIP) (Fig. 2a).…”