A Mn-N single-atom catalyst embedded in graphitic carbon nitride for efficient CO electroreduction.
Nat Commun
Beijing Key Laboratory of Ionic Liquids Clean Process, State Key Laboratory of Multiphase Complex Systems, Institute of Process Engineering, Chinese Academy of Sciences, 100190, Beijing, P.R. China.
Published: August 2020
Developing effective catalysts based on earth abundant elements is critical for CO electroreduction. However, simultaneously achieving a high Faradaic efficiency (FE) and high current density of CO (j) remains a challenge. Herein, we prepare a Mn single-atom catalyst (SAC) with a Mn-N site embedded in graphitic carbon nitride. The prepared catalyst exhibits a 98.8% CO FE with a j of 14.0 mA cm at a low overpotential of 0.44 V in aqueous electrolyte, outperforming all reported Mn SACs. Moreover, a higher j of 29.7 mA cm 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 site, which facilitates the formation of the key intermediate COOH through a lowered free energy barrier.
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| http://dx.doi.org/10.1038/s41467-020-18143-y | DOI Listing |
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