Tailoring oxygen vacancies in CoO yolk-shell nanospheres via for boosted peroxymonosulfate activation: Single-electron transfer and high-valent Co-oxo species-dominated non-radical pathways

Ta Cong KHIEM, Nguyen Nhat HUY, Eilhann KWON, Stanisław WACŁAWEK, Afshin EBRAHIMI, Wen-Da OH, Suresh GHOTEKAR, Yiu Fai TSANG , Wei-Hsin CHEN, Kun-Yi Andrew LIN

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4 Citations (Scopus)

Abstract

As CoO represents a promising material for peroxymonosulfate (PMS) activation, a yolk-shell-structured nanosphere, CoO₄‐x-0.20, is developed here for maximizing its catalytic activity by governing electronic structures via tailoring oxygen vacancies (OV) of CoO. This OV-tailored CoO enables single-electron transfer and generates high-valent cobalt-oxo species (Co(IV) = O) to achieve the fastest phenol degradation. The single-electron transfer is unraveled by an electron donation of Co atoms near OV to O to form O ̍¯ followed by O evolution after ¹O and the charge balance maintained by an electron acquisition from phenol by the electron-deficient Co atoms. Meanwhile, the generation of Co(IV) = O by the cleavage of the S—O bond in the Co(II)-O-SO-OH complex accepts electrons from phenol to turn back to Co(II) and Co(III), causing phenol oxidation. These results demonstrate the pre-eminence of CoO₄‐x-0.20 over the reported catalysts for phenol degradation and also offer insights into the mechanism of OV triggering electron donation and enhancing Co(IV) = O generation. Copyright © 2023 Elsevier B.V. All rights reserved.

Original languageEnglish
Article number146404
JournalChemical Engineering Journal
Volume476
Early online dateOct 2023
DOIs
Publication statusPublished - Nov 2023

Citation

Khiem, T. C., Huy, N. N., Kwon, E., Wacławek, S., Ebrahimi, A., Oh, W.-D., Ghotekar, S., Tsang, Y. F., Chen, W.-H., & Lin, K.-Y. A. (2023). Tailoring oxygen vacancies in Co₃O₄ yolk-shell nanospheres via for boosted peroxymonosulfate activation: Single-electron transfer and high-valent Co-oxo species-dominated non-radical pathways. Chemical Engineering Journal, 476, Article 146404. https://doi.org/10.1016/j.cej.2023.146404

Keywords

  • Phenol degradation
  • Co₃O₄
  • Oxygen vacancy
  • Single-electron transfer
  • High-valent cobalt-oxo species

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