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 N2 reduction offers a promising alternative to realize N2 fixation under ambient conditions. In this paper, PdP2 nanoparticles–reduced graphene oxide (PdP2–rGO) is proposed as an efficient electrocatalyst for the N2 reduction reaction. In 0.5 M LiClO4, PdP2–rGO affords a large NH3 yield rate of 30.3 μg h−1 mgcat.−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 μg h−1 mgcat.−1 and FE of 4.28%). This catalyst also shows high stability. Density functional theory calculations suggest that the barriers for N2 activation and the subsequent hydrogenation process on the Pd catalyst are alleviated after alloying with P.