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Synergistic effects in ordered Co oxides for boosting catalytic activity in advanced oxidation processes

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Hu,  Zhiwei
Zhiwei Hu, Physics of Correlated Matter, Max Planck Institute for Chemical Physics of Solids, Max Planck Society;

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Citation

Zhu, M., Guan, D., Hu, Z., Lin, H.-J., Chen, C.-T., Sheu, H.-S., et al. (2021). Synergistic effects in ordered Co oxides for boosting catalytic activity in advanced oxidation processes. Applied Catalysis B, 297: 120463, pp. 1-9. doi:10.1016/j.apcatb.2021.120463.


Cite as: https://hdl.handle.net/21.11116/0000-0008-E92B-2
Abstract
Synergistic effects are often used in catalyst design for many environmental/energy applications, however, the mechanism and a molecular-level structure to exert maximal synergy effects in catalyzing advanced oxidation processes (AOPs) in wastewater remediation are still unknown. Here, by designing a model perovskite family RBaCo2O6-δ (R = lanthanides) with Co4+ in octahedral coordination (Co4+ oct) and Co3+ in pyramidal coordination (Co3+ pyr), we ambitiously confirm the unique synergy of unsaturated (Co3+ pyr) and metallic (Co4+ oct) Co sites for efficient peroxymonosulfate (PMS) activation. Combined X-ray adsorption spectra and theoretical calculations strongly demonstrate that Co3+ pyr and Co4+ oct synergistically contribute to PMS adsorption and O[sbnd]O bond cleavage, and facilitate Co3+/Co4+ redox cycle for radical generation. With appropriate ratio and ordered distribution of Co3+ pyr/Co4+ oct, the Gd0.5La0.5BaCo2O5.75 exhibits remarkable catalytic activity for pollutant degradation, outperforming all previously reported Co4+-related oxides. This work may inspire rational design of efficient metal oxide catalysts. © 2021