Journal
CHINESE CHEMICAL LETTERS
Volume 32, Issue 5, Pages 1814-1818Publisher
ELSEVIER SCIENCE INC
DOI: 10.1016/j.cclet.2020.11.026
Keywords
Amorphous Co(OH)(2); Peroxymonosulfate (PMS); Acetaminophen (ACE); Intermediates; DFT calculation
Categories
Funding
- China Postdoctoral Science Foundation [2019M650007, 2020M670088]
- National Natural Science Foundation of China [21906001, 51721006]
- Beijing Nova Program [Z19111000110000]
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Amorphous Co(OH)(2) nanocages were found to be efficient in degrading acetaminophen (ACE) in wastewater, demonstrating superior removal capability and catalytic performance compared to crystalline beta-Co(OH)(2) and Co3O4. This study sheds light on the potential of using amorphous materials as heterogeneous catalysts in sulfate radicals-based advanced oxidation processes for the degradation of emerging organic contaminants.
Acetaminophen (ACE) is commonly used in analgesic and antipyretic drug, which is hardly removed by traditional wastewater treatment processes. Herein, amorphous Co(OH)(2) nanocages were explored as peroxymonosulfate (PMS) activator for efficient degradation of ACE. In the presence of amorphous Co (OH)(2) nanocages, 100% of ACE removal was reached within 2 min with a reaction rate constant k(1) = 3.68 min(-1) at optimum pH 5, which was much better than that of crystalline beta-Co(OH)(2) and Co3O4. Amorphous materials (disorder atom arrangement) with hollow structures possess large specific surface area, more reactive sites, and abundant vacancies structures, which could efficiently facilitate the catalytic redox reactions. The radicals quenching experiment demonstrated that SO4 center dot radicals dominated the ACE degradation rather than (OH)-O-center dot radicals. The mechanism of ACE degradation was elucidated by the analysis of degradation intermediates and theoretical calculation, indicating that the electrophilic SO4 center dot and (OH)-O-center dot tend to attack the atoms of ACE with high Fukui index (f ). Our finding highlights the remarkable advantages of amorphous materials as heterogeneous catalysts in sulfate radicals-based AOPs and sheds new lights on water treatment for the degradation of emerging organic contaminants. (C) 2021 Chinese Chemical Society and Institute of Materia Medica, Chinese Academy of Medical Sciences. Published by Elsevier B.V. All rights reserved.
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