Smart Interfacing between Co‐Fe Layered Double Hydroxide and Graphitic Carbon Nitride for High‐efficiency Electrocatalytic Nitrogen Reduction

Abstract

Bimetallic compounds such as hydrotalcite‐type layered double hydroxides (LDHs) are promising electrocatalysts owing to their unique electronic structures. However, their abilities toward nitrogen adsorption and reduction are undermined since the surface‐mantled, electronegative –OH groups hinder the charge transfer between transition metal atoms and nitrogen molecules. Herein, a smart interfacing strategy is proposed to construct a coupled heterointerface between LDH and 2D g‐C3N4, which is proven by density functional theory (DFT) investigations to be favorable for nitrogen adsorption and ammonia desorption compared with neat LDH surface. The interfaced LDH and g‐C3N4 is further hybridized with a self‐standing TiO2 nanofibrous membrane (NM) to maximize the interfacial effect owing to its high porosity and large surface area. Profited from the synergistic superiorities of the three components, the LDH@C3N4@TiO2 NM delivers superior ammonia yield (2.07 × 10−9 mol s−1 cm−2) and Faradaic efficiency (25.3%), making it a high‐efficiency, noble‐metal‐free catalyst system toward electrocatalytic nitrogen reduction.