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Interfacial hydrophobicity-induced desolvation effects on reductive dehalogenation by Zero-Valent Iron
Ke Pan1, Zekun Zhao1, Paul G Tratnyek2
1Zhejiang Key Laboratory of Low-carbon Control Technology for Industrial Pollution, College of Environment, Zhejiang University of Technology, Hangzhou 310014, China.
Modifying zero-valent iron (ZVI) with boron creates a hydrophobic surface. This enhances dehalogenation of polar contaminants like florfenicol by disrupting water interactions and increasing electron transfer efficiency.
Area of Science:
- Environmental Science
- Materials Science
- Chemistry
Background:
- Hydrophobic modifications of zero-valent iron (ZVI) improve non-polar contaminant reduction.
- The impact of hydrophobicity-driven desolvation on polar contaminant transformation by ZVI is not well understood.
Purpose of the Study:
- To comprehensively characterize the role of interfacial desolvation in enhancing ZVI-based dehalogenation.
- To investigate the effect of surface hydrophobicity on the dehalogenation of the amphiphilic pharmaceutical florfenicol (FF).
Main Methods:
- Preparation of ZVI with controlled hydrophobicity (sB-ZVI and B-ZVI) via mechanochemical boron introduction.
- Attenuated total reflection Fourier transform infrared (ATR-FTIR) analysis to study interfacial hydration and FF's CCl bond activation.
- Batch experiments with groundwater samples and aging tests to assess performance and stability.
Main Results:
- Hydrophobic BOx layer on sB-ZVI disrupts interfacial hydration, lowering FF's LUMO energy and increasing dehalogenation rates (2-5 fold).
- The BOx layer suppresses hydrogen evolution by approximately 80%.
- Overall electron efficiency (εe) increased by 38% for sB-ZVI compared to B-ZVI.
Conclusions:
- Interfacial desolvation is a key mechanism for enhancing ZVI performance in polar contaminant dehalogenation.
- Boron-modified ZVI (sB-ZVI) offers improved efficiency and stability for dehalogenation applications.
- Controlled surface hydrophobicity is a promising strategy for optimizing ZVI for environmental remediation.
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