Tungsten disulfide (WS2) is a highly active co-catalyst in Fe(III)/H2O2 Fenton-like reactions for efficient acetaminophen degradation
The most important factor that restricts the decomposition of H2O2 in the Fe3+/H2O2 reaction is the slow cycling efficiency of reducing Fe3+ to Fe2+. In this study, the addition of tungsten disulfide (WS2) as a co-catalyst achieved a rapid cycling of the reaction rate-limiting step and a significant...
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| Published in | The Science of the total environment Vol. 871; p. 162151 |
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| Main Authors | , , , , , , |
| Format | Journal Article |
| Language | English |
| Published |
Elsevier B.V
01.05.2023
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| Subjects | |
| Online Access | Get full text |
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| Abstract | The most important factor that restricts the decomposition of H2O2 in the Fe3+/H2O2 reaction is the slow cycling efficiency of reducing Fe3+ to Fe2+. In this study, the addition of tungsten disulfide (WS2) as a co-catalyst achieved a rapid cycling of the reaction rate-limiting step and a significant enhancement of H2O2 decomposition, which resulted in the effective degradation of acetaminophen (APAP). Results show that 99.6% of APAP (5 mg L−1) could be degraded by H2O2/Fe3+/WS2 system within 2.5 min. The conversion of Fe3+ to Fe2+ occurred mainly on the surface of WS2 due to the redox reaction of the exposed W4+ active sites with Fe3+ after the unsaturated S atoms were bound to protons. Electron paramagnetic resonance (EPR) and radical quenching experiments evaluated the contribution of hydroxyl radical (•OH) and superoxide radical (O2•−) in the degradation of pollutants. WS2 showed good recoverability after four cycles of the reaction. This study provides a new perspective to improve the efficiency of Fe3+/H2O2 and provides a reference for the involvement of transition metal sulfides in advanced oxidation processes (AOPs).
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•Addition of tungsten disulfide as a co-catalyst achieved a rapid Fe3+/Fe2+ cycling.•99.6 % of acetaminophen (5 mg L−1) could be degraded within 2.5 min by the system.•Fe3+/Fe2+ cycling was due to the redox reaction of exposed W4+ active site with Fe3+.•The contribution of hydroxyl radical (OH) and superoxide radical (O2−) was identified. |
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| AbstractList | The most important factor that restricts the decomposition of H₂O₂ in the Fe³⁺/H₂O₂ reaction is the slow cycling efficiency of reducing Fe³⁺ to Fe²⁺. In this study, the addition of tungsten disulfide (WS₂) as a co-catalyst achieved a rapid cycling of the reaction rate-limiting step and a significant enhancement of H₂O₂ decomposition, which resulted in the effective degradation of acetaminophen (APAP). Results show that 99.6% of APAP (5 mg L⁻¹) could be degraded by H₂O₂/Fe³⁺/WS₂ system within 2.5 min. The conversion of Fe³⁺ to Fe²⁺ occurred mainly on the surface of WS₂ due to the redox reaction of the exposed W⁴⁺ active sites with Fe³⁺ after the unsaturated S atoms were bound to protons. Electron paramagnetic resonance (EPR) and radical quenching experiments evaluated the contribution of hydroxyl radical (•OH) and superoxide radical (O₂•⁻) in the degradation of pollutants. WS₂ showed good recoverability after four cycles of the reaction. This study provides a new perspective to improve the efficiency of Fe³⁺/H₂O₂ and provides a reference for the involvement of transition metal sulfides in advanced oxidation processes (AOPs). The most important factor that restricts the decomposition of H2O2 in the Fe3+/H2O2 reaction is the slow cycling efficiency of reducing Fe3+ to Fe2+. In this study, the addition of tungsten disulfide (WS2) as a co-catalyst achieved a rapid cycling of the reaction rate-limiting step and a significant enhancement of H2O2 decomposition, which resulted in the effective degradation of acetaminophen (APAP). Results show that 99.6% of APAP (5 mg L−1) could be degraded by H2O2/Fe3+/WS2 system within 2.5 min. The conversion of Fe3+ to Fe2+ occurred mainly on the surface of WS2 due to the redox reaction of the exposed W4+ active sites with Fe3+ after the unsaturated S atoms were bound to protons. Electron paramagnetic resonance (EPR) and radical quenching experiments evaluated the contribution of hydroxyl radical (•OH) and superoxide radical (O2•−) in the degradation of pollutants. WS2 showed good recoverability after four cycles of the reaction. This study provides a new perspective to improve the efficiency of Fe3+/H2O2 and provides a reference for the involvement of transition metal sulfides in advanced oxidation processes (AOPs). [Display omitted] •Addition of tungsten disulfide as a co-catalyst achieved a rapid Fe3+/Fe2+ cycling.•99.6 % of acetaminophen (5 mg L−1) could be degraded within 2.5 min by the system.•Fe3+/Fe2+ cycling was due to the redox reaction of exposed W4+ active site with Fe3+.•The contribution of hydroxyl radical (OH) and superoxide radical (O2−) was identified. The most important factor that restricts the decomposition of H2O2 in the Fe3+/H2O2 reaction is the slow cycling efficiency of reducing Fe3+ to Fe2+. In this study, the addition of tungsten disulfide (WS2) as a co-catalyst achieved a rapid cycling of the reaction rate-limiting step and a significant enhancement of H2O2 decomposition, which resulted in the effective degradation of acetaminophen (APAP). Results show that 99.6% of APAP (5 mg L-1) could be degraded by H2O2/Fe3+/WS2 system within 2.5 min. The conversion of Fe3+ to Fe2+ occurred mainly on the surface of WS2 due to the redox reaction of the exposed W4+ active sites with Fe3+ after the unsaturated S atoms were bound to protons. Electron paramagnetic resonance (EPR) and radical quenching experiments evaluated the contribution of hydroxyl radical (•OH) and superoxide radical (O2•-) in the degradation of pollutants. WS2 showed good recoverability after four cycles of the reaction. This study provides a new perspective to improve the efficiency of Fe3+/H2O2 and provides a reference for the involvement of transition metal sulfides in advanced oxidation processes (AOPs).The most important factor that restricts the decomposition of H2O2 in the Fe3+/H2O2 reaction is the slow cycling efficiency of reducing Fe3+ to Fe2+. In this study, the addition of tungsten disulfide (WS2) as a co-catalyst achieved a rapid cycling of the reaction rate-limiting step and a significant enhancement of H2O2 decomposition, which resulted in the effective degradation of acetaminophen (APAP). Results show that 99.6% of APAP (5 mg L-1) could be degraded by H2O2/Fe3+/WS2 system within 2.5 min. The conversion of Fe3+ to Fe2+ occurred mainly on the surface of WS2 due to the redox reaction of the exposed W4+ active sites with Fe3+ after the unsaturated S atoms were bound to protons. Electron paramagnetic resonance (EPR) and radical quenching experiments evaluated the contribution of hydroxyl radical (•OH) and superoxide radical (O2•-) in the degradation of pollutants. WS2 showed good recoverability after four cycles of the reaction. This study provides a new perspective to improve the efficiency of Fe3+/H2O2 and provides a reference for the involvement of transition metal sulfides in advanced oxidation processes (AOPs). |
| ArticleNumber | 162151 |
| Author | Li, Jun Zeng, Ganning He, Dongqin Zeng, Yifeng Pan, Xiangliang Wang, Dongli Luo, Hongwei |
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| Snippet | The most important factor that restricts the decomposition of H2O2 in the Fe3+/H2O2 reaction is the slow cycling efficiency of reducing Fe3+ to Fe2+. In this... The most important factor that restricts the decomposition of H₂O₂ in the Fe³⁺/H₂O₂ reaction is the slow cycling efficiency of reducing Fe³⁺ to Fe²⁺. In this... |
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| SubjectTerms | acetaminophen Catalyst Decomposition disulfides electron paramagnetic resonance spectroscopy environment Ferric ion Hydrogen peroxide hydroxyl radicals Organics oxidation reaction kinetics superoxide anion tungsten |
| Title | Tungsten disulfide (WS2) is a highly active co-catalyst in Fe(III)/H2O2 Fenton-like reactions for efficient acetaminophen degradation |
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