A Mn-N<sub>3</sub> single-atom catalyst embedded in graphitic carbon nitride for efficient CO<sub>2</sub> electroreduction.
basic_science · Level V
Where this comes from
- Record sourced from PubMed, PMID 32859931.
- Also identified by DOI 10.1038/s41467-020-18143-y and PMC identifier 7455739.
- Licence recorded as CC BY.
- The licence permits redistribution, so the abstract is shown in full and the full text is available from the publisher.
Abstract
Developing effective catalysts based on earth abundant elements is critical for CO<sub>2</sub> electroreduction. However, simultaneously achieving a high Faradaic efficiency (FE) and high current density of CO (j<sub>CO</sub>) remains a challenge. Herein, we prepare a Mn single-atom catalyst (SAC) with a Mn-N<sub>3</sub> site embedded in graphitic carbon nitride. The prepared catalyst exhibits a 98.8% CO FE with a j<sub>CO</sub> of 14.0 mA cm<sup>-2</sup> at a low overpotential of 0.44 V in aqueous electrolyte, outperforming all reported Mn SACs. Moreover, a higher j<sub>CO</sub> of 29.7 mA cm<sup>-2</sup> is obtained in an ionic liquid electrolyte at 0.62 V overpotential. In situ X-ray absorption spectra and density functional theory calculations demonstrate that the remarkable performance of the catalyst is attributed to the Mn-N<sub>3</sub> site, which facilitates the formation of the key intermediate COOH<sup>*</sup> through a lowered free energy barrier.