PdP2 nanoparticles-reduced graphene oxide for electrocatalytic N2 conversion to NH3 under ambient conditions

Producing NH3 through the Haber-Bosch process has brought about huge energy-consumption and heavy emission of CO2. Electrochemical N-2 reduction offers a promising alternative to realize N-2 fixation under ambient conditions. In this paper, PdP2 nanoparticles-reduced graphene oxide (PdP2-rGO) is proposed as an efficient electrocatalyst for the N-2 reduction reaction. In 0.5 M LiClO4, PdP2-rGO affords a large NH3 yield rate of 30.3 mu g h(-1) mg(cat.)(-1) and a high faradaic efficiency of 12.56% at -0.1 V versus the reversible hydrogen electrode, which are much superior to those of its Pd-rGO counterpart (NH3 yield rate of 14.5 mu g h(-1) mg(cat.)(-1) and FE of 4.28%). This catalyst also shows high stability. Density functional theory calculations suggest that the barriers for N-2 activation and the subsequent hydrogenation process on the Pd catalyst are alleviated after alloying with P.