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Single-Atom Anchored Curved Carbon Surface for Efficient CO 2 Electro-Reduction with Nearly 100% CO Selectivity and Industrially-Relevant Current Density.
- Source :
-
Advanced materials (Deerfield Beach, Fla.) [Adv Mater] 2023 Sep; Vol. 35 (35), pp. e2205553. Date of Electronic Publication: 2023 Jul 13. - Publication Year :
- 2023
-
Abstract
- Although single metal atoms on porous carbons (PCs) are widely used in electrochemical CO <subscript>2</subscript> reduction reaction, these systems have long relied on flat graphene-based models, which are far beyond reality because of abundant curved structures in PCs; the effect of curved surfaces has long been ignored. In addition, the selectivity generally decreases under high current density, which severely limits practical application. Herein, theoretical calculations reveal that a single-Ni-atom on a curved surface can simultaneously enhance the total density of states around Fermi level and decrease the energy barrier for *COOH formation, thereby enhancing catalytic activity. This work reports a rational molten salt approach for preparing PCs with ultra-high specific surface area of up to 2635 m <superscript>2</superscript> g <superscript>-1</superscript> . As determined by cutting-edge techniques, a single Ni atom on a curved carbon surface is obtained and used as a catalyst for electrochemical CO <subscript>2</subscript> reduction. The CO selectivity reaches up to 99.8% under industrial-level current density of 400 mA cm <superscript>-2</superscript> , outperforming state-of-the-art PC-based catalysts. This work not only offers a new method for the rational synthesis of single atom catalysts with strained geometry to host rich active sites, but also provides in-depth insights for the origin of catalytic activity of curved structure-enriched PC-based catalysts.<br /> (© 2023 Wiley-VCH GmbH.)
Details
- Language :
- English
- ISSN :
- 1521-4095
- Volume :
- 35
- Issue :
- 35
- Database :
- MEDLINE
- Journal :
- Advanced materials (Deerfield Beach, Fla.)
- Publication Type :
- Academic Journal
- Accession number :
- 37365793
- Full Text :
- https://doi.org/10.1002/adma.202205553