Enhanced CO<sub>2</sub> Electrolysis Through Mn Substitution Coupled with Ni Exsolution in Lanthanum Calcium Titanate Electrodes.
basic_science · Level V
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- Record sourced from PubMed, PMID 37902720.
- Also identified by DOI 10.1002/adma.202308481.
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Abstract
In this study, perovskite oxides La<sub>0.3</sub>Ca<sub>0.6</sub>Ni<sub>0.05</sub>Mn<sub>x</sub>Ti<sub>0.95-</sub> <sub>x</sub>O<sub>3-</sub> <sub>γ</sub> (x = 0, 0.05, 0.10) are investigated as potential solid oxide electrolysis cell cathode materials. The catalytic activity of these cathodes toward CO<sub>2</sub> reduction reaction is significantly enhanced through the exsolution of highly active Ni nanoparticles, driven by applying a current of 1.2 A in 97% CO<sub>2</sub> - 3% H<sub>2</sub>O. The performance of La<sub>0.3</sub>Ca<sub>0.6</sub>Ni<sub>0.05</sub>Ti<sub>0.95</sub>O<sub>3-γ</sub> is notably improved by co-doping with Mn. Mn dopants enhance the reducibility of Ni, a crucial factor in promoting the in situ exsolution of metallic nanocatalysts in perovskite (ABO<sub>3</sub>) structures. This improvement is attributed to Mn dopants enabling more flexible coordination, resulting in higher oxygen vacancy concentration, and facilitating oxygen ion migration. Consequently, a higher density of Ni nanoparticles is formed. These oxygen vacancies also improve the adsorption, desorption, and dissociation of CO<sub>2</sub> molecules. The dual doping strategy provides enhanced performance without degradation observed after 133 h of high-temperature operation, suggesting a reliable cathode material for CO<sub>2</sub> electrolysis.