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Regulation of functional groups on graphene quantum dots directs selective CO2 to CH4 conversion.
- Source :
- Nature Communications; 9/6/2021, Vol. 12 Issue 1, p1-9, 9p
- Publication Year :
- 2021
-
Abstract
- A catalyst system with dedicated selectivity toward a single hydrocarbon or oxygenate product is essential to enable the industrial application of electrochemical conversion of CO<subscript>2</subscript> to high-value chemicals. Cu is the only known metal catalyst that can convert CO<subscript>2</subscript> to high-order hydrocarbons and oxygenates. However, the Cu-based catalysts suffer from diverse selectivity. Here, we report that the functionalized graphene quantum dots can direct CO<subscript>2</subscript> to CH<subscript>4</subscript> conversion with simultaneous high selectivity and production rate. The electron-donating groups facilitate the yield of CH<subscript>4</subscript> from CO<subscript>2</subscript> electro-reduction while electron-withdrawing groups suppress CO<subscript>2</subscript> electro-reduction. The yield of CH<subscript>4</subscript> on electron-donating group functionalized graphene quantum dots is positively correlated to the electron-donating ability and content of electron-donating group. The graphene quantum dots functionalized by either –OH or –NH<subscript>2</subscript> functional group could achieve Faradaic efficiency of 70.0% for CH<subscript>4</subscript> at −200 mA cm<superscript>−2</superscript> partial current density of CH<subscript>4</subscript>. The superior yield of CH<subscript>4</subscript> on electron-donating group- over the electron-withdrawing group-functionalized graphene quantum dots possibly originates from the maintenance of higher charge density of potential active sites (neighboring C or N) and the interaction between the electron-donating group and key intermediates. This work provides insight into the design of active carbon catalysts at the molecular scale for the CO<subscript>2</subscript> electro-reduction. Electrochemical conversion of CO<subscript>2</subscript> to fuels is a promising strategy to reduce the ever-increasing CO<subscript>2</subscript> emission. Here, the authors developed graphene quantum dots (GQDs) catalysts to efficiently convert CO<subscript>2</subscript> to CH<subscript>4</subscript> and revealed the significance of electron-donating functional groups in regulating the reactivity of GQDs. [ABSTRACT FROM AUTHOR]
- Subjects :
- QUANTUM groups
QUANTUM dots
FUNCTIONAL groups
METAL catalysts
GRAPHENE
Subjects
Details
- Language :
- English
- ISSN :
- 20411723
- Volume :
- 12
- Issue :
- 1
- Database :
- Complementary Index
- Journal :
- Nature Communications
- Publication Type :
- Academic Journal
- Accession number :
- 152296650
- Full Text :
- https://doi.org/10.1038/s41467-021-25640-1