Synergistic electrocatalytic N2 reduction using a PTCA nanorod–rGO hybrid. Issue 20 (9th May 2019) - Li, Peipei
Abstract : As a non-noble-metal electrocatalyst for the N2 reduction reaction, a perylene-3, 4, 9, 10-tetracarboxylic acid nanorod-reduced graphene oxide hybrid offers a large NH3 yield of 24.7 μg h −1 mgcat. −1 with a high faradaic efficiency of 6.9%. Abstract : 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, a perylene-3, 4, 9, 10-tetracarboxylic acid nanorod-reduced graphene oxide (PTCA–rGO) nanohybrid is proposed as a metal-free electrocatalyst to synergistically enhance 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 mgcat. −1 and a high faradaic efficiency of 6.9% at −0.50 V vs. the reversible hydrogen electrode, which are much superior to those of PTCA and rGO counterparts. This catalyst also shows a high electrochemical and structural stability. Density functional theory calculations suggest that the NRR over the hybrid catalyst takes place via both distal associative and partially alternative routes.