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Atomically Dispersed Manganese on Carbon Substrate for Aqueous and Aprotic CO 2 Electrochemical Reduction.
- Source :
-
Advanced materials (Deerfield Beach, Fla.) [Adv Mater] 2023 Mar; Vol. 35 (12), pp. e2210658. Date of Electronic Publication: 2023 Feb 07. - Publication Year :
- 2023
-
Abstract
- CO <subscript>2</subscript> utilization and conversion are of great importance in alleviating the rising CO <subscript>2</subscript> concentration in the atmosphere. Here, a single-atom catalyst (SAC) is reported for electrochemical CO <subscript>2</subscript> utilization in both aqueous and aprotic electrolytes. Specifically, atomically dispersed Mn-N <subscript>4</subscript> sites are embedded in bowl-like mesoporous carbon particles with the functionalization of epoxy groups in the second coordination spheres. Theoretical calculations suggest that the epoxy groups near the Mn-N <subscript>4</subscript> site adjust the electronic structure of the catalyst with reduced reaction energy barriers for the electrocatalytic reduction of CO <subscript>2</subscript> to CO. The resultant Mn-single-atom carbon with N and O doped catalyst (MCs-(N,O)) exhibits extraordinary electrocatalytic performance with a high CO faradaic efficiency of 94.5%, a high CO current density of 13.7 mA cm <superscript>-2</superscript> , and a low overpotential of 0.44 V in the aqueous environment. Meanwhile, as a cathode catalyst for aprotic Li-CO <subscript>2</subscript> batteries, the MCs-(N,O) with well-regulated active sites and unique mesoporous bowl-like morphology optimizes the nucleation behavior of discharge products. MCs-(N,O)-based batteries deliver a low overpotential and excellent cyclic stability of 1000 h. The findings in this work provide a new avenue to design and fabricate SACs for various electrochemical CO <subscript>2</subscript> utilization systems.<br /> (© 2023 Wiley-VCH GmbH.)
Details
- Language :
- English
- ISSN :
- 1521-4095
- Volume :
- 35
- Issue :
- 12
- Database :
- MEDLINE
- Journal :
- Advanced materials (Deerfield Beach, Fla.)
- Publication Type :
- Academic Journal
- Accession number :
- 36641734
- Full Text :
- https://doi.org/10.1002/adma.202210658