Semi-metallic reconfiguration induced by asymmetrically interatomic-interactions accelerate electrochemical nitrate reduction

Abstract

Effective conversion from nitrate to ammonia using an electrochemical method is attracting much attention, but which has to face the difficulty of lower conversion performance and unavoidable competing reaction. Herein, we develop an intriguing surface engineering strategy to reorganize orderly the electronic structures of catalysts, in which the superficial Cu sites can be asymmetrically hybridized with internal Fe atoms through an indirect orbital interaction, finally leading to a semi-metallic characteristic to optimize the adsorption or dissociation process of nitrates. The comprehensive calculations confirm that the potential barriers at the rate-limiting steps can be effectively decreased due to their appropriate bonding interaction with reactants. More importantly, the competing hydrogen evolution reaction is also suppressed. This work suggests a feasible strategy to accelerate nitrate reduction by particular catalyst surface engineering.