Asymmetric Chemical Potential Activated Nanointerfacial Electric Field for Efficient Vanadium Redox Flow Batteries

ACS Nano. 2023 Nov 14;17(21):21799-21812. doi: 10.1021/acsnano.3c07732. Epub 2023 Oct 20.

Abstract

Constructing active sites with enhanced intrinsic activity and accessibility in a confined microenvironment is critical for simultaneously upgrading the round-trip efficiency and lifespan of all-vanadium redox flow battery (VRFB) yet remains under-explored. Here, we present nanointerfacial electric fields (E-fields) featuring outstanding intrinsic activity embodied by binary Mo2C-Mo2N sublattice. The asymmetric chemical potential on both sides of the reconstructed heterogeneous interface imposes the charge movement and accumulation near the atomic-scale N-Mo-C binding region, eliciting the configuration of an accelerator-like E-field from Mo2N to Mo2C sublattice. Supported with theoretical calculations and intrinsic activity tests, the improved vanadium ion adsorption behavior and charge-transfer process at the nanointerfacial sites were further substantiated, hence expediting the electrochemical kinetics. Accordingly, the pronounced promotion is achieved in the resultant flow battery, yielding an energy efficiency of 77.7% and an extended lifespan of 1000 cycles at 300 mA cm-2, outperforming flow cells with conventional single catalysts in most previous reports.

Keywords: Nanointerfacial electric field; adsorption behavior; asymmetric chemical potential; charge transfer process; intrinsic activity.