Plasma Chemical Looping: Unlocking High-Efficiency CO<sub>2</sub> Conversion to Clean CO at Mild Temperatures



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.

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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