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

Aqueous Zn-ion batteries hold practical promise for large-scale energy storage because of the safety and affordability of aqueous-based electrolytes; in addition, the manufacturing process is significantly simplified by direct employment of Zn metal as an anode. However, hydrogen evolution due to near-surface water dissociation has hindered large-scale applications of them. Here, we report the suppression of the hydrogen evolution reaction via a CuN 3 -coordinated graphitic carbonitride (CuN 3 -C 3 N 4 ) anticatalytic interface to achieve highly efficient aqueous Zn-ion batteries. Based on in situ gas chromatography and in situ synchrotron-based X-ray diffraction spectroscopy, we demonstrated that the hydrogen evolution reaction triggers the Zn 4 SO 4 (OH) 6 · x H 2 O formation. A combination of in situ infrared spectroscopy and density functional theory simulations has proved to stabilize near-surface H 3 O + species and regulate adsorption of H* intermediates by an anticatalytic interface for hydrogen evolution reaction suppression. Consequently, the anticatalytic interface greatly improves the Coulombic efficiency of Zn plating/stripping to ∼99.7% for 5500 cycles and the cycling reversibility to over 1300 h at 1 mA cm -2 and 1 mAh cm -2 . With an anticatalytic interface, the full cell shows an excellent Coulombic efficiency of 98.3% over 400 cycles at 1C. These findings provide strategic insight for targeted designing of highly efficient aqueous Zn-ion batteries.