Citation: Jizhou Jiang, Lianglang Yu, Fangyi Li, Wenming Deng, Cong Pan, Haitao Wang, Jing Zou, Yaobin Ding, Fengxia Deng, Jia Huang. Water Steam Bathed FeS₂ for Highly Efficient Fenton Degradation of Alachlor[J]. Acta Physico-Chimica Sinica, ;2023, 39(3): 220903. doi: 10.3866/PKU.WHXB202209033 shu

Water Steam Bathed FeS₂ for Highly Efficient Fenton Degradation of Alachlor

Jizhou Jiang ¹ ,
Lianglang Yu ¹ ,
Fangyi Li ¹ ,
Wenming Deng ¹ ,
Cong Pan ² ,
Haitao Wang ^1,, ,
Jing Zou ¹ ,
Yaobin Ding ² ,
Fengxia Deng ³ ,
Jia Huang ^1,,

1.
School of Environmental Ecology and Biological Engineering, School of Chemistry and Environmental Engineering, School of Chemical Engineering and Pharmacy, Key Laboratory of Green Chemical Engineering Process of Ministry of Education, Engineering Research Center of Phosphorus Resources Development and Utilization of Ministry of Education, Novel Catalytic Materials of Hubei Engineering Research Center, Wuhan Institute of Technology, Wuhan 430205, China
2.
College of Resources and Environmental Science, South-Central Minzu University, Wuhan 430074, China
3.
State Key Laboratory of Urban Water Resources and Environment, School of Environment, Harbin Institute of Technology, Harbin 150090, China

Corresponding author: Haitao Wang, wanghaitao@wit.edu.cn Jia Huang, 21070201@wit.edu.cn
Received Date: 21 September 2022
Revised Date: 14 October 2022
Accepted Date: 25 October 2022
Available Online: 31 October 2022
Fund Project: the National Natural Science Foundation of China 62004143the National Natural Science Foundation of China 21876209Key R & D Program of Hubei Province, China 2022BAA084Natural Science Foundation of Hubei Province, China 2021CFB133the Central Government Guided Local Science and Technology Development Special Fund Project, China 2020ZYYD033the Open Research Fund of Key Laboratory of Material Chemistry for Energy Conversion and Storage, China (HUST), Ministry of Education, China 2021JYBKF05the Innovation Project of Engineering Research Center of Phosphorus Resources Development and Utilization of Ministry of Education, China LCX2021003the Opening Fund of Key Laboratory for Green Chemical Process of Ministry of Education of Wuhan Institute of Technology, China GCP202101

Fenton-like activity of iron sulfides for the generation of reactive oxygen species and degradation of various organic pollutants has been extensively investigated due to its abundance in the natural environment. However, their Fenton-like activity is usually unsatisfactory due to the limited exposure of surface ferrous reactive sites. In this work, a new strategy to enhance the Fenton-like activity of iron sulfides, using pyrite (FeS₂) as a model, was developed based on the heat treatment of FeS₂ by water steam. It was found that the FeS₂ heat-treated by water steam (Heat-FeS₂) exhibited much higher heterogeneous Fenton activity in the degradation of alachlor (ACL) than its parent FeS₂ prepared from hydrothermal reaction (Fresh-FeS₂). At an initial pH of 6.3, the rate of degradation of ACL by Heat-FeS₂ Fenton system was 0.48 min⁻¹, which is ~23 times higher than that of Fresh-FeS₂ Fenton system. Electron spin resonance analysis and benzoic acid probe experiments confirmed the production of more hydroxyl (•OH) and superoxide radicals (•O₂⁻) in Heat-FeS₂ Fenton system than Fresh-FeS₂ Fenton system. The increased Fenton-like activity of Heat-FeS₂ can be attributed to the increased content of highly reactive surface bonded Fe²⁺/Fe³⁺ species, higher amount of leached Fe²⁺, and optimal reaction pH due to stronger acidification of Heat-FeS₂. Characterization studies by scanning electron microscopy, transmission electron microscopy, X-ray photoelectron spectroscopy (XPS), and Fourier-transform infrared spectroscopy showed that heat treatment remarkably promoted the transformation of lattice Fe²⁺ to surface reactive Fe²⁺, allowing the exposure of more surface reactive Fe²⁺ and leaching of Fe²⁺; simultaneously, heat treatment enhanced the generation of surface SO₄²⁻, creating a highly acidic surface. The surface Fe²⁺ percentage in the surface total iron was raised from 13% in Fresh-FeS₂ to 29% in Heat-FeS₂. Fe²⁺ leaching from Heat-FeS₂ was 0.23 mmol·L⁻¹, much higher than that (< 0.02 mmol·L⁻¹) for Fresh-FeS₂. The change in the surface Fe and S species in the Heat-FeS₂ system during the Fenton-like reaction was monitored by XPS to elucidate the enhanced Fenton oxidation mechanism. The characterization results showed that after Fenton reaction with H₂O₂, the surface contents of Fe²⁺ and Fe³⁺ species on Fresh-FeS₂ and Heat-FeS₂ were remarkably raised, while the surface content of S₂²⁻ species was reduced, confirming the crucial role of S₂²⁻ in the reductive cycle of Fe³⁺ to Fe²⁺. These findings increase understanding of the oxidative transformation and corrosion of iron sulfides and its relevant transformation and degradation of toxic organics in natural environments. The results of this work also provide an efficient Fenton-like oxidation method based on iron sulfides for highly efficient degradation of organic pollutants (e.g. ACL) in aqueous solution.
- FeS₂,
- Water steam treatment,
- Fenton,
- Surface Fe²⁺ species,
- Alachlor
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Water Steam Bathed FeS₂ for Highly Efficient Fenton Degradation of Alachlor