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可迁移性零价铁的制备及其活化过硫酸盐氧化修复石油污染土壤
引用本文:王兴族,王茂林,王亚玲,柴旭辉,蔡喜运.可迁移性零价铁的制备及其活化过硫酸盐氧化修复石油污染土壤[J].环境科学研究,2023,36(1):89-99.
作者姓名:王兴族  王茂林  王亚玲  柴旭辉  蔡喜运
作者单位:大连理工大学环境学院,工业生态与环境工程教育部重点实验室,辽宁 大连 116024
基金项目:国家重点研发计划项目(No.2019YFC1803803);国家自然科学基金项目(No.21976025)
摘    要:纳米零价铁(nZVI)活化过硫酸盐(PS)体系具有活性高、持效性长等潜在优势,在有机污染土壤修复领域具有良好的应用前景.然而,nZVI颗粒易于发生团聚和被空气氧化,在土壤中迁移性能和稳定性能较差,限制了其活化性能的发挥.本研究采用聚天冬氨酸(PASP)修饰和硫化改性技术,制备了可迁移的零价铁复合材料(PASP-S-nZVI),评价了PASP-S-nZVI的活化PS性能及其在石英砂填充介质中的迁移性能,优化了该材料活化PS降解土壤中石油烃的反应条件,并开展了土壤污染修复小试试验. SEM-EDS和XPS表征结果显示,PASP-S-nZVI材料为表面具有PASP涂层及硫铁化物(FeSx)的零价铁.与未改性nZVI和S-nZVI相比,PASP-S-nZVI材料的悬浮稳定性、Zeta电位和电子利用率都显著增加,表明双重改性增加了nZVI的稳定性能.柱试验结果显示,PASP-S-nZVI具有较低的附着效率,其实际碰撞效率是S-nZVI的38.0%、nZVI的26.5%,在含水介质中的迁移性能显著增加,且增加程度与填充介质的粒径尺寸和水体pH有关.在优化的条件参数下,PASP...

关 键 词:聚天冬氨酸  硫化纳米零价铁  过硫酸盐  氧化  石油烃
收稿时间:2022-05-22

Preparation of Mobile PASP-S-Zero-Valent Iron Materials for Persulfate Remediation of Petroleum Contaminated Soils
Affiliation:Key Laboratory of Industrial Ecology and Environmental Engineering (Ministry of Education), School of Environmental Science and Technology, Dalian University of Technology, Dalian 116024, China
Abstract:Persulfates (PS) are mainstream oxidants used to remediate soils contaminated with organic pollutants such as petroleum hydrocarbons. Nano zero-valent iron (nZVI) is a well-known persulfate activator, which has the advantages of high catalytic reaction and long-term performance. However, nZVI is prone to agglomeration and oxidation processes in soils and has poor stability and migration potential, both of which inhibit the activation potential of nZVI. In this study, a mobile zero-valent iron composite material (PASP-S-nZVI) was prepared by modifying nZVI with polyaspartic acid (PASP) and sodium hydrosulfite, and quartz sand column experiments of PASP-S-nZVI and remediation experiments of petroleum-contaminated soils by PASP-S-nZVI/PS were carried out. The SEM-EDS and XPS spectra of materials showed that the PASP-S-nZVI composite materials had characteristics of nZVI with both PASP coating layer and FeSx layer on the surface. The combined modifications resulted in reduction of total iron contents in the composite materials, but a notable increase in the stability of materials due to the increases in zeta potential and specific surface area of the materials. The results of the column experiments showed that PASP-S-nZVI had low attachment efficiency, and its actual single-collector removal efficiency was 38.0% of that of S-nZVI and 26.5% of that of nZVI. It indicated that the migration performance of PASP-S-nZVI in aqueous media increased significantly, which depends on the particle sizes of the packing media and water pH. Under optimized conditions, PASP-S-nZVI/PS efficiently removed petroleum hydrocarbons (TPHs) in soils, and the removal rate of TPHs (3 d) was 77%±2% in the laboratory experiments. The pilot-scale experiment also yielded a high removal rate of 53%±2% of TPHs (3 d), further indicating the performance of PASP-S-nZVI/PS in soils. This study indicates that PASP-S-nZVI with improved mobility and catalytic reactivity may have applications in soil remediation. 
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