Honeycomb-like porous 3D nickel electrodeposition for stable Li and Na metal anodes

Abstract

Li and Na metals have the highest theoretical anode capacity for Li/Na batteries, but the operational safety hazards stemming from uncontrolled growth of Li/Na dendrites and unstable electrode-electrolyte interfaces hinder their real-world applications. Recently, the emergence of 3D conductive scaffolds aimed at mitigating the dendritic growth to improve the cycling stability has gained traction. However, while achieving 3D scaffolds that are conducive to completely prevent dendritic Li/Na is challenging, the routes proposed to fabricate 3D scaffolds to date are often complex and expensive. This not only leads to sub-optimal battery performance but can make the manufacturing nearly unachievable, compromising their commercial viability. We herein introduce a facile and single-step route to honeycomb-like 3D porous Ni@Cu scaffolds via a hydrogen bubble dynamic template (HBDT) electrodeposition method. The current collectors fabricated by this method offer highly stable cycling performance of Li plating/stripping (>300 cycles at 0.5 mAh cm⁻² and over 200 cycles at 1.0 mAh cm⁻²), attributed to their ability to effectively accommodate Li/Na deposits in their porous networks and to delocalize the charge distribution. The beneficial role of LiNO₃ as an electrolyte additive in improving the mechanical integrity of solid electrolyte interface (SEI) and mechanistic insights into how the 3D porous structure facilitates Li/Na plating/stripping are comprehensively presented. Finally, with an outstanding cycling performance of reversible Na deposition (over 240, 110 and 50 cycles for 0.5, 1.0 and 2.0 mAh cm⁻² at 1.0 mA cm⁻²), our findings open new doors to expedite the development of Li/Na metal battery technology.