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- Title
Selective CO<sub>2</sub>‐to‐CO Conversion Enabled by Ultrathin Nitrogen‐Modified Graphene Confined Cobalt–Cobalt Oxide Nanocomposites with Prominent Electron Synergy.
- Authors
Bi, Qingyuan; Luo, Rui; Zeng, Mengqi; Deng, Xinyue; Wang, Jinyu; Hao, Weiju; Hu, Keyan; Fan, Jinchen; Li, Guisheng; Huang, Fuqiang
- Abstract
Developing and fabricating cost‐effective materials for efficient thermocatalytic reduction of CO2 to CO under mild conditions is a promising and practical way to sustainable and green low‐carbon energy systems, which remains a challenge. Herein, a facile high‐temperature pyrolysis strategy for the synthesis of efficient ultrathin nitrogen‐modified graphene confined cobalt oxide (CoOx@NG) nanocomposites with prominent electron synergistic effect on inner Co─CoO core and confinement of N‐modified graphene shell is reported. The electronic and/or geometric structures of active metallic Co and coordinatively unsaturated CoO species are modulated by the graphene confinement effect. The electron‐rich N dopant in the graphene shell enhances the surface electron density of the catalyst, thus regulating the adsorption of acidic CO2 molecules. The engineered CoOx@NG shows an outstanding selective CO2‐to‐CO efficiency, with a conversion of 19.5% and a near full CO selectivity at 523 K as well as excellent stability for 150 h on stream. Moreover, the in‐depth insights into the material microstructure, electron synergy, structure‐activity relationships, key intermediate species, and a three‐step reaction mechanism involving the rate‐determining step of C═O bond cleavage for critical *C═O species via 13CO2 isotope and in situ spectroscopy are also demonstrated.
- Subjects
GRAPHENE; NANOCOMPOSITE materials; STRUCTURE-activity relationships; ELECTRON density; ELECTRONS
- Publication
Advanced Functional Materials, 2024, Vol 34, Issue 24, p1
- ISSN
1616-301X
- Publication type
Article
- DOI
10.1002/adfm.202315079