In situ destruction of halogenated Superfund contaminants with persulfate-generated radicals

用过硫酸盐产生的自由基原位破坏卤化超级基金污染物

• 批准号: 10349971
• 负责人: David L. Sedlak
• 金额: $ 26.84万
• 依托单位: UNIVERSITY OF CALIFORNIA BERKELEY
• 依托单位国家: 美国
• 财政年份: 1997
• 资助国家: 美国
• 起止时间: 1997-04-01 至 2027-06-30
• 项目状态: 未结题
• 来源: https://reporter.nih.gov/project-details/10349971
• 关键词: Address; Alcohols; Aldehydes; Ames Assay; Anaerobic Bacteria; Biological Assay; Bioremediations; Carbon; Chemicals; Chronic; Collaborations; Community Health; Complex; Cysteine; Dose; Ecosystem; Engineering; Environment; Estrogens; Ethers; Exhibits; Film; Flushing; Glutathione; Hazardous Waste Sites; Hexachlorobenzene; Histidine; Hydrocarbons; Hydrogen Peroxide; Hydrophobicity; Hydroxyl Radical; In Situ; Ketones; Lysine; Mass Fragmentography; Metabolic Biotransformation; Methods; Modeling; Mutagenicity Tests; Nucleic Acids; Organic solvent product; Oxidants; Oxidation-Reduction; Oxidative Stress; Oxygen; Permeability; Petroleum; Phase; Poison; Polybrominated Biphenyls; Polychlorinated Biphenyls; Predisposition; Process; Production; Property; Pump; Reaction; Reducing Agents; Research; Resistance; Risk; Sampling; Signal Recognition Particle; Site; Soil; Solid; Solvents; Source; Sulfate; Sulfhydryl Compounds; Superfund; System; Techniques; Temperature; Testing; Toxic effect; Water Supply; acute toxicity; aqueous; cold temperature; drinking water; estrogenic activity; experience; ground water; high throughput screening; kinetic model; liquid chromatography mass spectrometry; novel; novel strategies; organic acid; organic contaminant; oxidation; parental monitoring; pollutant; predictive modeling; remediation; screening; superfund site

PROJECT 4: SUMMARY/ABSTRACT After 40 years of research and field experience, the remediation of hazardous waste sites remains a substantial challenge. Over the past three decades, considerable progress has been made in the use of in situ treatment methods, such as bioremediation and permeable reactive barriers. Nonetheless, excavation and off-site disposal remains the most common remedial approach for soil and groundwater extraction (i.e., pump-and-treat) systems are still being employed at numerous Superfund sites. Among the emerging alternatives to these expensive approaches, in situ chemical oxidation (ISCO) has shown substantial potential for providing an effective means of remediating a variety of contaminants, including TCE and petroleum hydrocarbons. Despite its popularity, ISCO has proven difficult to use in the treatment of hydrophobic compounds and compounds that exhibit low reactivity towards hydroxyl radical and sulfate radical—the two strongest oxidants produced during the decomposition of hydrogen peroxide and peroxydisulfate (i.e., persulfate) in the subsurface. Our proposed research aims at developing new in situ chemical remediation techniques capable of treating Superfund contaminants that often require expensive ex-situ methods, (fully halogenated organic solvents, polychlorinated biphenyl (PCBs), polybrominated biphenyl ethers (PBDEs), and per- and polyfluorinated alkyl substances (PFAS)) by employing Anaerobic Radical Treatment (ART). In Aim 1, we propose to develop and optimize anaerobic thermally activated persulfate methods to dehalogenate recalcitrant contaminants. We will develop a kinetic model that will account for temperature, pH, oxidant dose, contaminant concentration, and oxygen concentration. In Aim 2, we will develop a method that employs the use of co-solvent flushing followed by ART. In anaerobic conditions, activated persulfate can react with alcohols to form carbon centered radicals that are able to degrade contaminants. We also predict that persulfate can activate at lower temperature in the presence of solvents, which will allow for more efficient treatment of complex chemical mixtures. This includes aqueous film-forming foams (AFFF) used at sites contaminated with halogenated solvents. Aim 3 is focused on the discovery and fate of stable transformation products formed during ART. In collaboration with Project 3, we will investigate biodegradability of transformation products in microcosm studies. Aim 4 focuses on predicting possible modes of toxicity by utilizing computational toxicity models, screening with biomolecule assays, as well as established bioassay such as the Ames test. The results of Project 4 could provide novel approaches for the remediation of highly halogenated emerging and legacy compounds in the environment, while providing new models and methods for minimizing toxic transformation products.

项目4：摘要/摘要 经过40年的研究和现场经验，修复有害废物 站点仍然是一个重大挑战。在过去的三十年中，取得了很大的进步 是在使用原位治疗方法（例如生物修复和可渗透的）中制作的 反应性障碍。尽管如此，开挖和场外处置仍然是最常见的 土壤和地下水提取（即泵和治疗）系统的补救方法仍在 在众多超级基金网站担任雇员。在这些新兴替代方案中 昂贵的方法，原位化学氧化（ISCO）已显示出很大的潜力 提供一种有效的方法来修复各种污染物，包括TCE和 石油烃。尽管它很受欢迎，但事实证明，ISCO很难在 疏水化合物和化合物的处理，使低反应性暴露于 hydroxyl radical and sulfate radical—the two strong oxideants produced during the 地下表面中过氧化氢和过氧二硫酸盐（即过硫酸盐）的分解。 我们提出的研究旨在开发能够的新的原位化学补救技术 处理通常需要昂贵的前坐标方法的超级基金污染物（完全 卤代有机溶液，多氯联苯（PCB），多溴双苯基醚 （PBDES），以及使用厌氧菌的烷基物质（PFAS）） 激进治疗（ART）。 在AIM 1中，我们建议开发和优化厌氧热活化的过硫酸盐 去盐酸恢复污染物的方法。我们将开发一个动力学模型 考虑温度，pH，氧化剂量，污染物浓度和氧气 专注。在AIM 2中，我们将开发一种采用使用共迎接冲洗的方法 其次是艺术。在厌氧条件下，活化的硫酸盐可以与醇反应形成 能够降解污染物的碳为中心的自由基。我们还预测这是过人的 在存在溶液的情况下可以在较低温度下激活，这将允许更有效 treatment of complex chemical mixtures.这包括使用水性膜泡沫（AFFF） 在被卤化溶液污染的地点。 AIM 3专注于发现和命运 艺术期间形成的稳定转换产品。与项目3合作，我们将 在缩影研究中研究转化产物的生物降解性。 AIM 4专注于 通过使用计算毒性模型来预测可能的毒性模式 生物分子测定以及已建立的生物测定法，例如AMES测试。结果 项目4可以提供新颖的方法来修复高度卤素的新兴 和环境中的遗产化合物，同时提供新的模型和方法 最小化有毒的转化产品。