4.7 Article

Hierarchical nano-vesicles with bimetal-encapsulated for peroxymonosulfate activation: Singlet oxygen-dominated oxidation process

期刊

CHEMICAL ENGINEERING JOURNAL
卷 433, 期 -, 页码 -

出版社

ELSEVIER SCIENCE SA
DOI: 10.1016/j.cej.2021.133581

关键词

Hierarchical nano-vesicle; Bimetal-encapsulated; Peroxymonosulfate activation; Singlet oxygen

资金

  1. National Natural Science Foundation of China [51878335, 52070095]
  2. Natural Science Foundation of Jiangsu province [BK20191255]

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In this study, hierarchical nano-vesicles with bimetal-encapsulated FeCu1.5O3 were designed for peroxymonosulfate activation. The FeCu1.5O3 was encapsulated in hollow zeolite spheres to enhance the contact with reactants. The bimetal oxide surface improved the affinity with adsorbates and accelerated electron transfer. The results showed that the bimetal oxide-loaded hierarchical nano-vesicles could efficiently generate singlet oxygen for organic degradation.
Hierarchical nano-vesicles with bimetal-encapsulated (FeCu1.5O3@NV) was designed for peroxymonosulfate (PMS) activation with the( 1)O(2)-dominated oxidation process. Different from previous core-shell metal-loaded catalysts, FeCu1.5O3 was encapsulated in hollow zeolite spheres, and these zeolite sphere units assembled to construct hierarchical nano-vesicles. Owning to mesoporous shell and abundant interior cavity, FeCu1.5O3@NV could enrich reactants in cavity for enhancing the contact with active sites. The flexible surface of bimetal oxides strengthened the affinity with surface adsorbates and substrates, accelerating the electron transfer between re-actants. DFT calculation indicated that FeCu1.5O3@NV possessed strong binding affinity for BPA and PMS, facilitating PMS activation and BPA degradation inside of hollow sphere units. Being attributed to the synergistic effect of bimetal redox couples and hierarchical nano-vesicle structure, large amounts of O-1(2) could be generated through two pathways for BPA degradation. The first pathway is the reaction between bimetal redox couples and PMS, and the second is the chain reaction of O2 & BULL;-. Due to bimetal oxides uniformly encapsulated in hierarchical nano-vesicles,FeCu1.5O3@NV possessed high catalytic stability with negligible metal leaching. Even after 5 cycles, BPA removal could still remain 100%.

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