Suppressing Hydrogen Evolution via Anticatalytic Interfaces toward Highly Efficient Aqueous Zn-Ion Batteries

Area of Science:

• Materials Science
• Electrochemistry
• Energy Storage

Background:

• Aqueous zinc-ion batteries (AZIBs) offer safe and affordable energy storage solutions.
• However, hydrogen evolution reaction (HER) from water dissociation limits their practical application.
• Zinc metal anode instability due to HER hinders AZIB performance.

Purpose of the Study:

• To suppress the hydrogen evolution reaction (HER) in AZIBs.
• To enhance the Coulombic efficiency and cycling stability of AZIBs.
• To provide insights into designing stable AZIBs.

Main Methods:

• Fabrication of a CuN3-coordinated graphitic carbonitride (CuN3-C3N4) anticatalytic interface.
• In situ gas chromatography and synchrotron-based X-ray diffraction spectroscopy to study HER.
• In situ infrared spectroscopy and density functional theory (DFT) simulations to understand reaction mechanisms.

Main Results:

• The CuN3-C3N4 interface effectively suppressed HER, preventing Zn4SO4(OH)6·xH2O formation.
• Stabilization of near-surface H3O+ and regulation of H* adsorption by the anticatalytic interface.
• Achieved high Coulombic efficiency (~99.7% for 5500 cycles) for Zn plating/stripping.
• Demonstrated long cycling reversibility (>1300 h) and excellent full-cell performance (98.3% efficiency over 400 cycles).

Conclusions:

• The CuN3-C3N4 anticatalytic interface is a promising strategy for suppressing HER in AZIBs.
• This approach significantly improves the Coulombic efficiency and cycling stability of AZIBs.
• The findings offer valuable guidance for the rational design of high-performance aqueous zinc-ion batteries.