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A Mn single atom catalyst with Mn–N2O2 sites integrated into carbon nanosheets for efficient electrocatalytic CO2 reduction.
- Source :
- Journal of Materials Chemistry A; 5/28/2022, Vol. 10 Issue 20, p10892-10901, 10p
- Publication Year :
- 2022
-
Abstract
- The electrocatalytic reduction of CO<subscript>2</subscript> using electricity produced from renewable resources is a strategy for achieving CO<subscript>2</subscript> emission reduction and sustainable energy development. Further, the reaction has a large number of industrial practical applications, since CO<subscript>2</subscript> can be converted to fuels via downstream chemical processing of the CO product. Herein, we successfully synthesized a low Mn-content single-atom catalyst (SAC) with Mn–N<subscript>2</subscript>O<subscript>2</subscript> sites, covalently integrated into carbon nanosheets (Mn–NO/CNs) using a one-pot synthesis method. The Mn–NO/CN catalyst displays efficient electrocatalytic performance for the CO<subscript>2</subscript> reduction reaction (CO<subscript>2</subscript>RR). Using an H-type electrolytic cell, the maximum CO Faraday efficiency (FE) at −0.460 V (V vs. RHE) reaches 96.0% in 0.5 M KHCO<subscript>3</subscript> electrolyte. In the flow cell measurements, Mn–NO/CNs exhibits a current density of 28 mA cm<superscript>−2</superscript> at a very low potential of −0.425 V (V vs. RHE) for the CO<subscript>2</subscript>RR with 1.0 M KOH as the mobile phase. The FE<subscript>CO</subscript> remains above 80% even after 70 h, demonstrating the excellent durability of the catalyst even at a very low potential. The X-ray absorption spectra (XAS) and DFT calculations show that the Mn–N<subscript>2</subscript>O<subscript>2</subscript> site is the active catalytic center, which facilitates the adsorption of CO<subscript>2</subscript> and significantly lowers the free energy barrier leading to the formation of the critical intermediate *COOH. The presence of dual N and O coordinated to the single atom metal sites embedded in the 2D carbon nanosheet significantly improves catalytic activity for the reduction of CO<subscript>2</subscript>. Therefore, the catalytic performance of the single atom metal catalyst can be enhanced by adjusting the coordination environment. [ABSTRACT FROM AUTHOR]
Details
- Language :
- English
- ISSN :
- 20507488
- Volume :
- 10
- Issue :
- 20
- Database :
- Complementary Index
- Journal :
- Journal of Materials Chemistry A
- Publication Type :
- Academic Journal
- Accession number :
- 173555181
- Full Text :
- https://doi.org/10.1039/d2ta01285e