Boosting Electroreduction of Nitrate and CO<sub>2</sub> to Urea on a Tandem Fe<sub>1</sub>/MoS<sub>2</sub> Catalyst.
basic_science · Level V
Where this comes from
- Record sourced from PubMed, PMID 39312392.
- Also identified by DOI 10.1021/acsnano.4c10187.
- No licence information is recorded for this record.
- Because redistribution is not established, this page shows the abstract only. Follow the links below for the full text.
Abstract
Urea electrosynthesis by coelectrolysis of NO<sub>3</sub><sup>-</sup> and CO<sub>2</sub> (UENC) holds enormous promise for sustainable urea production, while the efficient UENC process relies on the rational design of high-performance catalysts to facilitate the electrocatalytic C-N coupling efficiency and the hydrogenation reaction process. Herein, Fe single atoms supported on MoS<sub>2</sub> (Fe<sub>1</sub>/MoS<sub>2</sub>) are developed as a highly effective and robust catalyst for UENC. Theoretical calculations and operando spectroscopic measurements reveal a tandem catalysis mechanism of the Fe<sub>1</sub>-S<sub>3</sub> motif and MoS<sub>2</sub>-edge to jointly promote the UENC process, where the Fe<sub>1</sub>-S<sub>3</sub> motif drives the early C-N coupling and subsequent *CO<sub>2</sub>NO<sub>2</sub>-to-*CO<sub>2</sub>NH<sub>2</sub> step. The generated *CO<sub>2</sub>NH<sub>2</sub> is then migrated from the Fe<sub>1</sub>-S<sub>3</sub> motif to the nearby MoS<sub>2</sub>-edge, which facilitates the *CO<sub>2</sub>NH<sub>2</sub> → *COOHNH<sub>2</sub> step for urea formation. Noticeably, Fe<sub>1</sub>/MoS<sub>2</sub> assembled in a flow cell reaches a maximum urea Faraday efficiency of 54.98% with a corresponding urea yield rate of 18.98 mmol h<sup>-1</sup> g<sup>-1</sup>, performing at the top level among all of the UENC catalysts reported to date.