Synergistically electrocatalytic N2 reduction by PTCA nanorod-rGO hybrid

Currently, industrial-scale NH3 production mainly relies on the energy-intensive and CO2-emitting Haber-Bosch process from atmospheric N2 and fossil fuels. Electrochemical N2 fixation offers an eco-friendly and sustainable alternative to ambient NH3 synthesis with the aid of efficient electrocatalysts for the N2 reduction reaction (NRR). Here, perylene-3,4,9,10-tetracarboxylic acid nanorod-reduced graphene oxide (PTCA-rGO) nanohybrid is proposed as a metal-free electrocatalyst to synergistically enhance the N2 reduction under ambient reaction conditions. In 0.1 M HCl, the PTCA-rGO hybrid provides a large NH3 yield of 24.7 µg h–1 mg–1cat. and a high Faradic efficiency of 6.9% at –0.50 V vs. reversible hydrogen electrode, much superior to PTCA and rGO counterparts. This catalyst also shows high electrochemical and structure stability. Density functional theory calculations suggest that the NRR over the hybrid catalyst takes place via both distal associative and partially alternative routes.