CO<sub>2</sub>-mediated porphyrin catalysis in reversible Li-CO<sub>2</sub> cells
- Authors
- Kim, Boran; Shin, Kihyun; Henkelman, Graeme; Ryu, Won-Hee
- Issue Date
- Dec-2023
- Publisher
- ELSEVIER SCIENCE SA
- Citation
- CHEMICAL ENGINEERING JOURNAL, v.477
- Journal Title
- CHEMICAL ENGINEERING JOURNAL
- Volume
- 477
- URI
- https://scholarworks.sookmyung.ac.kr/handle/2020.sw.sookmyung/159514
- DOI
- 10.1016/j.cej.2023.147141
- ISSN
- 1385-8947
1873-3212
- Abstract
- Li-CO2 cells provide exceptional benefit by storing considerable energy and achieving environmental carbon fixation. However, the sluggish kinetics of the Li-CO2 reaction and severe cell polarization with low efficiency must be addressed. Here, we show that the manganese phthalocyanine (MnPc) molecule, a porphyrin-based homogeneous catalyst, significantly reduces the overpotential (similar to 50 %) and improves Li-CO2 cell performance during prolonged cycling. The reversible Li-CO2 reaction pathway proceeding via a LixCO2 intermediate species and catalyzed by MnPc was examined by in situ characterization and first principles calculations. We reveal the structural changes occurring in the MnPc catalyst with metal-to-ligand charge transfer when the electrochemically reduced CO2*- radical intermediate is bound to the Mn center after discharge; consequently, the reverse reaction enables recharging. This study introduces a way to understand and design organometallic homogeneous catalysts involving CO2 mediation of environmental energy storage systems and carbon negative.
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