(544e) Highly Selective Electrochemical Reduction of CO2 to CO Via a Novel Catalyst with Mn-N3 Site | AIChE

(544e) Highly Selective Electrochemical Reduction of CO2 to CO Via a Novel Catalyst with Mn-N3 Site


Feng, J. - Presenter, Laboratory
Zeng, S., Chinese Academy of Sciences
Zhang, S., Beijing Key Laboratory of Ionic Liquids Clean Process,CAS Key Labroratory of Green Process and Engineering, Institute of Process Engineering, Chinese Academy of Sciences
Zhang, X., Institute of Process Engineering, Chinese Academy
Electrochemical CO2 reduction reaction (CO2RR) is one of the most promising ways to deal with the excess CO2 and resolve the energy crisis [1]. However, due to the stability of CO2 molecule and reaction involves multiple electrons and protons, poor selectivity and low current density are the main challenges of this filed [2]. So, efficient catalysts are in great need.

As the third abundance of transition metals in Earth’s crust, manganese (Mn) has shown great potentials on many electrocatalytic fields. Nevertheless, the performance of Mn based catalysts is largely limited for CO2RR. Herein, we firstly prepared Mn single-atom catalyst (SAC) with Mn-N3 site supported by g-C3N4. The prepared catalyst exhibited a maximum CO FE of 98.8% with 14.0 mA cm-2 CO current density (jCO) at overpotential of 0.44 V in KHCO3 electrolyte, outperforming all reported Mn SACs and being one of the best reported electrocatalysts for CO2 conversion CO. Moreover, a higher jCO value of 29.7 mA cm-2 was obtained at overpotential of 0.62 V, when ionic liquid was used as electrolyte. In-situ experiment and DFT results confirmed that Mn-N3 site is the active site, on which the free energy barrier of key intermediate formation is greatly reduced. It can be anticipated that Mn SACs may also exhibit excellent performance in other electrochemical reactions through changing supporting materials to form exclusive active site.


[1] Feng JQ, Gao HS, Feng JP, Liu L, Zeng SJ, Dong HF, Bai YG, Liu LC, Zhang XP. Morphology modulation‐engineered flowerlike In2S3 via ionothermal method for efficient CO2 Electroreduction. ChemCat Chem, 2020, 12: 926-931.

[2] Feng JP, Zeng SJ, Liu HZ, Feng JQ, Gao HS, Bai L, Dong HF, Zhang SJ, Zhang XP. Insights into carbon dioxide electroreduction in ionic liquids: Carbon dioxide activation and selectivity tailored by ionic microhabitat. ChemSusChem, 2018, 11: 3191-3197.