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

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 x 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.