Multi-component gradients in 3D host frameworks enabled stack-type zinc plating/stripping for highly durable aqueous...

Area of Science:

• Materials Science
• Electrochemistry
• Energy Storage

Background:

• Developing dendrite-free zinc metal anodes is crucial for high-durability aqueous zinc-ion batteries.
• Existing methods face challenges in controlling zinc deposition and preventing side reactions.

Purpose of the Study:

• To propose an in situ constructed 3D restrained host framework with multi-component gradients.
• To enable controllable and rapid stack-type zinc plating/stripping behavior for enhanced battery performance.

Main Methods:

• Fabrication of a 3D host framework (g'-Ag/g-PSiOx-NH2/CP) using amino-functionalized polysilane and silver nanoparticles on a carbon paper scaffold.
• Investigating the gradient effects on zinc ion desolvation and deposition.
• Testing symmetric cells and Zn||MnO2 full batteries.

Main Results:

• The g'-Ag/g-PSiOx-NH2/CP electrodes demonstrated high Coulombic efficiency and long cyclability (>5000 hours at 10 mA cm-2/10 mAh cm-2).
• Zn||MnO2 full batteries achieved a specific capacity of 200.1 mAh g-1 with 82.2% retention after 800 cycles.
• Large-size pouch batteries showed good rate capability and cyclability with high-loading cathodes.

Conclusions:

• The developed 3D framework effectively induces controlled zinc plating/stripping with a 'first-in/last-out' mode.
• This scalable strategy offers a feasible solution for high-durability rechargeable metal-based batteries.
• The approach significantly advances the development of stable and long-lasting aqueous zinc-ion batteries.