Single-Atom Catalysts Dispersed on Graphitic Carbon Nitride (g-CN): Eley–Rideal-Driven CO-to-Ethanol Conversion
The electrochemical reduction of carbon monoxide (COER) offers a promising route for generating value-added multi-carbon (C<sub>2+</sub>) products, such as ethanol, but achieving high catalytic performance remains a significant challenge. Herein, we performed comprehensive density functi...
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| Main Authors: | , , , , |
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| Format: | Article |
| Language: | English |
| Published: |
MDPI AG
2025-07-01
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| Series: | Nanomaterials |
| Subjects: | |
| Online Access: | https://www.mdpi.com/2079-4991/15/14/1111 |
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| Summary: | The electrochemical reduction of carbon monoxide (COER) offers a promising route for generating value-added multi-carbon (C<sub>2+</sub>) products, such as ethanol, but achieving high catalytic performance remains a significant challenge. Herein, we performed comprehensive density functional theory (DFT) computations to evaluate CO-to-ethanol conversion on single metal atoms anchored on graphitic carbon nitride (TM/g–CN). We showed that these metal atoms stably coordinate with edge N sites of g–CN to form active catalytic centers. Screening 20 TM/g–CN candidates, we identified V/g–CN and Zn/g–CN as optimal catalysts: both exhibit low free-energy barriers (<0.50 eV) for the key <sup>*</sup>CO hydrogenation steps and facilitate C–C coupling via an Eley–Rideal mechanism with a negligible kinetic barrier (~0.10 eV) to yield ethanol at low limiting potentials, which explains their superior COER performance. An analysis of d-band centers, charge transfer, and bonding–antibonding orbital distributions revealed the origin of their activity. This work provides theoretical insights and useful guidelines for designing high-performance single-atom COER catalysts. |
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| ISSN: | 2079-4991 |