MoO3 nanosheets for efficient electrocatalytic N2 fixation to NH3

TLDR: In this article, a non-noble-metal MoO3 nanosheets act as an efficient nonnoble metal catalyst for electrochemical N2 fixation to NH3 with excellent selectivity at room temperature and atmospheric pressure.

Abstract: The synthesis of NH3 heavily depends on the energy-intensive Haber–Bosch process with a large amount of greenhouse gas emission. Electrochemical reduction offers a carbon-neutral process to convert N2 to NH3 at ambient conditions, but requires efficient and stable catalysts for the N2 reduction reaction. Mo-dependent nitrogenases and synthetic molecular complexes have attracted increasing attention for N2 fixation; however, less attention has been paid to Mo-based nanocatalysts for electrochemical N2 conversion to NH3. Herein, we report that MoO3 nanosheets act as an efficient non-noble-metal catalyst for electrochemical N2 fixation to NH3 with excellent selectivity at room temperature and atmospheric pressure. In 0.1 M HCl, this catalyst exhibits remarkable NRR activity with an NH3 yield of 4.80 × 10−10 mol s−1 cm−2 (29.43 μg h−1 mgcat.−1) and a faradaic efficiency of 1.9%. Moreover, this catalyst also shows high electrochemical stability and durability. Density functional theory calculations reveal that the outermost Mo atoms serve as the active sites for effective N2 adsorption.