Synergistic Single-Atom Ru and Mof-Derived Oxygen Vacancy Zro2-Porous Carbon to Boost the Efficiency for Electrochemical Nitrogen Fixation

Abstract

Ammonia is an important raw material for chemical, fertilizer, and energy storage. Energy-intensive industrial nitrogen fixation goes against the carbon-neutral concept and needs to be replaced by clean alternative electrochemical nitrogen fixation methods (ENF). Herein, we report a single-atom Ru loaded on MOF-derived oxygen-rich vacancies ZrO2 porous carbon material (Ru@ ZrO-PL) by plasma etching technique to enhance the ENF properties with the NH3 yield rate of 83.1 ± 2.4 μg h−1 mgcat−1 and the Faradaic efficiency (FE) of 13.8 ± 0.4 at -0.25 V vs RHE. The advanced flow cell device improves the efficiency of material transfer and greatly enhances the ENF properties of the Ru@ ZrO-PL, with an NH3 yield rate up to 113.1 ± 6.5 μg h−1 mgcat−1 and FE up to 57.3 ± 2.9% at -0.20 V vs RHE. This work provides new ideas for enhancing the ENF performance of single-atom materials and highlights the advantages of novel devices.

Keywords: electrochemical nitrogen fixation, single atoms, Ru, MOF-derived carbon, flow cell