Atomic-Level Customization of Zinc Crystallization Kinetics at the Interface for High-Utilization Zn Anodes

Area of Science:

• Materials Science
• Electrochemistry
• Surface Chemistry

Background:

• Achieving high reversibility in zinc anodes is critical for battery performance.
• Controlling crystallization at interfaces during electrochemical deposition remains a challenge.
• Atomic-scale design rules for crystallization kinetics lack predictive power.

Purpose of the Study:

• To develop a crystal facet terminating agent for modulating zinc deposition.
• To understand the role of synergistic ion adsorption in regulating zinc growth kinetics.
• To enhance the reversibility and performance of zinc anodes.

Main Methods:

• Interface molecular dynamics (MD) simulations.
• Experimental electrochemical deposition.
• Analysis of adsorption free energy and ion aggregation.

Main Results:

• LaCl3 was identified as a crystal facet terminating agent.
• Synergistic adsorption of La3+ and Cl- ions controlled Zn crystallization.
• A strong (002) facet texture of Zn deposits was achieved.
• Zn anodes demonstrated high cumulative capacity (12 Ah cm-2 at 40 mA cm-2).
• Zn||MnO2 full cells maintained practical areal capacity (3.39 mAh cm-2).

Conclusions:

• LaCl3 effectively modulates Zn deposition orientation by regulating growth kinetics.
• The developed agent significantly enhances zinc anode reversibility and performance.
• The findings show promise for practical applications in high-energy-density batteries.
• Successful scale-up to a 0.34 Ah pouch cell validates the approach.