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A Mn-N3 single-atom catalyst embedded in graphitic carbon nitride for efficient CO2 electroreduction.

ABSTRACT: Developing effective catalysts based on earth abundant elements is critical for CO2 electroreduction. However, simultaneously achieving a high Faradaic efficiency (FE) and high current density of CO (jCO) remains a challenge. Herein, we prepare a Mn single-atom catalyst (SAC) with a Mn-N3 site embedded in graphitic carbon nitride. The prepared catalyst exhibits a 98.8% CO FE with a jCO of 14.0?mA?cm-2 at a low overpotential of 0.44?V in aqueous electrolyte, outperforming all reported Mn SACs. Moreover, a higher jCO of 29.7?mA?cm-2 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-N3 site, which facilitates the formation of the key intermediate COOH* through a lowered free energy barrier.

SUBMITTER: Feng J 

PROVIDER: S-EPMC7455739 | biostudies-literature | 2020 Aug

REPOSITORIES: biostudies-literature

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A Mn-N<sub>3</sub> single-atom catalyst embedded in graphitic carbon nitride for efficient CO<sub>2</sub> electroreduction.

Feng Jiaqi J   Gao Hongshuai H   Zheng Lirong L   Chen Zhipeng Z   Zeng Shaojuan S   Jiang Chongyang C   Dong Haifeng H   Liu Licheng L   Zhang Suojiang S   Zhang Xiangping X  

Nature communications 20200828 1

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 aque  ...[more]

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