Citation: Juanjuan Qi, Juzhe Liu, Fengbin Sun, Taobo Huang, Jun Duan, Wen Liu. High active amorphous Co(OH)₂ nanocages as peroxymonosulfate activator for boosting acetaminophen degradation and DFT calculation[J]. Chinese Chemical Letters, ;2021, 32(5): 1814-1818. doi: 10.1016/j.cclet.2020.11.026 shu

High active amorphous Co(OH)₂ nanocages as peroxymonosulfate activator for boosting acetaminophen degradation and DFT calculation

Juanjuan Qi ^{a, b} ,
Juzhe Liu ^c ,
Fengbin Sun ^{b, d} ,
Taobo Huang ^{b, d} ,
Jun Duan ^{b, d} ,
Wen Liu ^{b, d, *,}

a.
The Key Laboratory of Resources and Environmental Systems Optimization, Ministry of Education, College of Environmental Science and Engineering, North China Electric Power University, Beijing 102206, China
b.
The Key Laboratory of Water and Sediment Sciences, Ministry of Education, College of Environmental Sciences and Engineering, Peking University, Beijing 100871, China
c.
School of Chemistry and Beijing Advanced Innovation Center for Biomedical Engineering, Beihang University, Beijing 100191, China
d.
State Environmental Protection Key Laboratory of All Material Fluxes in River Ecosystems, Peking University, Beijing 100871, China

wen.liu@pku.edu.cn

Received Date: 17 September 2020
Revised Date: 19 October 2020
Accepted Date: 13 November 2020
Available Online: 20 November 2020

Figures(5)

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 k₁ = 3.68 min^-1 at optimum pH 5, which was much better than that of crystalline β-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^·- radicals dominated the ACE degradation rather than ^·OH radicals. The mechanism of ACE degradation was elucidated by the analysis of degradation intermediates and theoretical calculation, indicating that the electrophilic SO₄^·- and ^·OH 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.
- Amorphous Co(OH)₂,
- Peroxymonosulfate (PMS),
- Acetaminophen (ACE),
- Intermediates,
- DFT calculation
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High active amorphous Co(OH)2 nanocages as peroxymonosulfate activator for boosting acetaminophen degradation and DFT calculation

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High active amorphous Co(OH)₂ nanocages as peroxymonosulfate activator for boosting acetaminophen degradation and DFT calculation