Electrochemical Performance of Diamond-like Carbon (DLC)-Coated Zn Anodes for Application to Aqueous Zinc-Ion Batteries

Abstract

The increasing demand for safe, cost-effective, and sustainable energy storage solutions has spotlighted aqueous zinc-ion batteries (AZIBs) as promising alternatives to lithium-ion systems. However, the practical deployment of AZIBs remains hindered by dendritic growth, hydrogen evolution, and surface corrosion at the zinc metal anode, which severely compromise electrochemical stability. In this study, we propose an interfacial engineering strategy involving ultrathin diamond-like carbon (DLC) coatings applied to Zn anodes. The DLC films serve as conformal, ion-permeable barriers that mitigate parasitic side reactions and facilitate uniform Zn plating/stripping behavior. Materials characterizations of the DLC layer on the Zn anodes revealed the tunability of sp(2)/sp(3) hybridization and surface morphology depending on DLC thickness. Electrochemical impedance spectroscopy demonstrated a significant reduction in interfacial resistance, particularly in the optimally coated sample (DLC2, similar to 20 nm), which achieved a favorable balance between mechanical integrity and ionic transport. Symmetric-cell tests confirmed enhanced cycling stability over 160 h, while full-cell configurations with an ammonium vanadate nanofiber-based cathode exhibited superior capacity retention over 900 cycles at 2 A g(-1). The DLC2-coated Zn anodes demonstrated the most effective performance, attributable to its moderate surface roughness, reduced disorder, and minimized charge-transfer resistance. These results provide insight into the importance of fine-tuning the DLC thickness and carbon bonding structure for suppressing dendrite formation and enhancing electrochemical stability.