(Invited) N2 Reduction to NH3 Generation Using Transition Metal-Based Catalysts

Abstract

We use 2D transition metal dichalcogenide (TMDC) catalysts and MoO2 nanoparticles to facilitate the N2 reduction to NH3 via dark electrocatalysis. Transition metal-based catalysts offer a unique opportunity to exploit the d electrons and orbitals for N2 activation. Specifically, the 2D TMDC catalysts are highly tunable 2D catalysts, where the band energetics, surface functionalization, defects, and phase can be tuned to control the N2 reactivity to generate NH3. We use indophenol and 1H NMR with isotope labeling to identify NH3 from the catalytic reaction and not from setup/system contaminants. Through various attempts and iterations, we have many lessons learned about experimental setup that will be communicated. Moreover via a collaboration with Professor Thoi’s Group at Johns Hopkins, we used defect-rich MoO2 nanoparticles interfaced with carbon nanowires to achieve high NH3 yields (21.2 mg h-1 mg-1) and Faradaic efficiencies (> 30%). This work will be summarized where we characterized the catalyst with a variety of X-ray spectroscopic techniques.