Long, Yanhui, Wang, Xingzi, Zhang, Hai, Wang, Kaiyi, Ong, Wee-Liat, Bogaerts, Annemie, Li, Kongzhai, Lu, Chunqiang, Li, Xiaodong, Yan, Jianhua et al (show 2 more authors)
(2024)
Plasma Chemical Looping: Unlocking High-Efficiency CO<sub>2</sub> Conversion to Clean CO at Mild Temperatures.
JACS Au, 4 (7).
pp. 2462-2473.
Abstract
We propose a plasma chemical looping CO<sub>2</sub> splitting (PCLCS) approach that enables highly efficient CO<sub>2</sub> conversion into O<sub>2</sub>-free CO at mild temperatures. PCLCS achieves an impressive 84% CO<sub>2</sub> conversion and a 1.3 mmol g<sup>-1</sup> CO yield, with no O<sub>2</sub> detected. Crucially, this strategy significantly lowers the temperature required for conventional chemical looping processes from 650 to 1000 °C to only 320 °C, demonstrating a robust synergy between plasma and the Ce<sub>0.7</sub>Zr<sub>0.3</sub>O<sub>2</sub> oxygen carrier (OC). Systematic experiments and density functional theory (DFT) calculations unveil the pivotal role of plasma in activating and partially decomposing CO<sub>2</sub>, yielding a mixture of CO, O<sub>2</sub>/O, and electronically/vibrationally excited CO<sub>2</sub>*. Notably, these excited CO<sub>2</sub>* species then efficiently decompose over the oxygen vacancies of the OCs, with a substantially reduced activation barrier (0.86 eV) compared to ground-state CO<sub>2</sub> (1.63 eV), contributing to the synergy. This work offers a promising and energy-efficient pathway for producing O<sub>2</sub>-free CO from inert CO<sub>2</sub> through the tailored interplay of plasma and OCs.
| Item Type: | Article |
|---|---|
| Uncontrolled Keywords: | 34 Chemical Sciences, 3406 Physical Chemistry, 7 Affordable and Clean Energy |
| Divisions: | Faculty of Science and Engineering > School of Electrical Engineering, Electronics and Computer Science |
| Depositing User: | Symplectic Admin |
| Date Deposited: | 13 May 2024 07:55 |
| Last Modified: | 09 Aug 2024 12:44 |
| DOI: | 10.1021/jacsau.4c00153 |
| Open Access URL: | https://doi.org/10.1021/jacsau.4c00153 |
| Related URLs: | |
| URI: | https://livrepository.liverpool.ac.uk/id/eprint/3180897 |
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