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Effective removal of Sb(V) from aqueous solutions by micro-electrolysis with composite scrap iron-manganese as filler

以废铁锰为填料的微电解技术高效除锑研究

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Abstract

Micro-electrolysis (ME) technology is investigated for improving the efficiency of removal of pentavalent antimony (Sb(V)) from the environment. In this study, an ME system composed of scrap iron filings, waste manganese fillings, and activated carbon (Fe-Mn-C ME) was used to efficiently remove Sb(V). The results proved that, compared with conventional iron-carbon micro-electrolysis (Fe-C ME), Fe-Mn-C ME significantly enhances the removal rate of Sb(V) when the hydraulic retention time is 10–24 h. The Fe-Mn flocs produced by this system were analyzed using X-ray diffraction (XRD), energy-dispersive X-ray spectroscopy (EDS), X-ray photoelectron spectroscopy (XPS), and Brunauer-Emmett-Teller (BET) surface area analysis, which revealed that the flocs were mostly Mn-substituted FeOOH and had a relatively larger specific surface area, providing better adsorption performance. Furthermore, it was found that the removal rate of Sb(V) decreased as the iron-carbon mass ratio increased, while it first increased and then decreased as the manganese content increased. The reduction of Fe(III) was accelerated with an increase in the addition of manganese, leading to an increase in the concentration of Fe(II). The electron transfer and the formation of Fe(II) were facilitated by the potential difference between manganese and carbon, as well as by the formation of microcells between iron and manganese, which improved the reduction ability of Sb(V). From our thorough investigation and research, this is the first report that has proposed Fe-Mn-C ME for removing antimony. It provides a novel approach and technological support for removing Sb(V) efficiently.

摘要

目的

近年来锑污染日益严重, 因此亟需探索出经济有效的方法除锑。本文旨在提出一种经济环保、操作简单、效果稳定的微电解除锑技术, 并探究其去除效果、影响因素及去除机理。

创新点

1. 提出了基于铁锰碳填料的微电解系统除锑;2. 探究了铁锰碳微电解体系除锑的主要机理(包括氧化还原作用、吸附和共沉淀作用)。

方法

1. 在不同水力停留时间、铁碳质量比和锰含量的情况下, 探究铁锰碳微电解去除性能的变化;2. 对微电解产生的絮体进行X射线衍射、能量色散X射线光谱、比表面积测试、X射线光电子能谱等微观结构分析, 探究铁锰复合双氢氧化物的形成和Sb(V)去除的机理。

结论

1. 当水力停留时间为10~24 h、填料投加量为250 g/L、pH值为6.5、铁碳比为1.6:1、Sb(V)初始浓度为1 mg/L时, 铁锰碳微电解的Sb(V)平均去除率比铁碳微电解高7.60%~9.67%。2. 最佳实验工况下, 铁锰碳微电解法的Sb(V)去除率可达91.85%。3. 机理分析表明, 在铁锰碳微电解反应中, 部分Sb(V)被反应生成的具有良好吸附性能的铁锰复合双氢氧化物絮体吸附去除, 而另一部分被还原为Sb(III), 并在混凝过程中生成Sb(OH)3沉淀, 进而被絮体的吸附和共沉淀反应去除。

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Acknowledgments

This work is supported by the National Key R&D Program of China (No. 2019YFC0408400) and the National Natural Science Foundation of China (No. 51878597).

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Authors

Contributions

All authors contributed to the study conception and design. Shangkun DING: conceptualization; investigation; writing–original draft preparation. Saihua HUANG: supervision; writing–reviewing and editing. Yiping ZHANG: methodology; supervision. Yongchao ZHOU: conceptualization; methodology.

Corresponding author

Correspondence to Yongchao Zhou  (周永潮).

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Shangkun DING, Saihua HUANG, Yiping ZHANG, and Yongchao ZHOU declare that they have no conflict of interest.

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Tables S1–S5, Figs. S1 and S2, Section S1

Electronic Supplementary Material

11582_2024_552_MOESM1_ESM.pdf

Electronic Supplementary Materials: Effective removal of Sb(V) from aqueous solutions by micro-electrolysis with composite scrap iron-manganese as filler

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Ding, S., Huang, S., Zhang, Y. et al. Effective removal of Sb(V) from aqueous solutions by micro-electrolysis with composite scrap iron-manganese as filler. J. Zhejiang Univ. Sci. A (2024). https://doi.org/10.1631/jzus.A2300287

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  • DOI: https://doi.org/10.1631/jzus.A2300287

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