In situ destruction of halogenated Superfund contaminants with biological radical reactions

项目3：总结/摘要 高度卤化的化合物包括最近认识到的污染物，例如全氟化烷基和多氟化烷基。 以及遗留污染物，如氯化溶剂、多氯联苯 （多氯联苯）和多溴联苯醚（多溴二苯醚）。PFAS和其他极持久性卤化 化合物并不单独存在于场所中。例如，氯化溶剂（例如，三氯乙烯）经常共存 与1，4-二氧六环和PFAS以及包括苯和二甲苯在内的燃料成分。高度卤化 即使共污染物已得到补救，化合物仍留在场地中， 通过饮用水源和食物接触对人体受体的健康风险。作为更高 卤化化学品的发现，修复策略需要结合联合收割机选择性和高 反应性几十年来，生物修复一直是有吸引力的，由于选择性酶靶向特定的 污染物。同样，化学氧化还原处理由于其高反应性而引起了人们的兴趣。但 在自然界和化学处理后的恶劣场地条件下， 这两种技术在单独应用时都有缺点。产生自由基的生物酶系统是 广泛存在于需氧和厌氧环境中的微生物系统中。我们假设这些生物- 自由基系统可能成为一种新的修复方法，结合了选择性和高 反应性 在目标1中，我们建议采用生物信息学和分子生物学技术来研究已知的和假定的 在高通量测定中使用多种化学介体化合物的漆酶系统来确定优化的 PFAS治疗系统。目标2侧重于研究厌氧自由基系统的反应，如 甘氨酰自由基酶（GRE）和S-腺苷甲硫氨酸（SAM），以研究其未来的工程能力 补救战略。我们将在目标3中结合联合收割机项目3和4的方法，其中化学处理将 用于引发污染物，使其更适合随后的生物彻底处理，以及 研究了化学处理前后微生物群落动态。项目3的结果可以 提供一种新的补救技术方法，以补救新出现和遗留的高卤化 环境中的化合物，以保护周围社区的环境健康。

PROJECT 3: SUMMARY/ABSTRACT Highly halogenated compounds include recently recognized pollutants such as per- and polyfluorinated alkyl substances (PFAS) as well as legacy contaminants, such as chlorinated solvents, polychlorinated biphenyls (PCBs) and Polybrominated diphenyl ethers (PBDEs). PFAS and other extremely persistent halogenated compounds do not exist alone in sites. For example, chlorinated solvents (e.g., trichloroethylene) often coexist with 1,4-dioxane and PFAS, as well as fuel components including benzene and xylene. Highly halogenated compounds remain in sites even when co-contaminants have been remediated, posing continued environmental health risks to human receptors through exposure via drinking water sources and food. As more highly halogenated chemicals are discovered, remediation strategies need to combine both selectivity and high reactivity. For decades bioremediation has been attractive due to selective enzymes targeting specific contaminants. Likewise, chemical redox treatment has garnered interest due to its high reactivity. However, it takes decades to evolve new specific enzymes in nature and the harsh site conditions after chemical treatment are drawbacks to both technologies when applied alone. Biological enzymatic systems that produce radicals are widespread in microbial systems in aerobic and anaerobic environments. We hypothesize that these biological- radical systems could become a novel remediation approach that combines both selectivity and high reactivity. In Aim 1, we propose to employ bioinformatics and molecular biology techniques to study known and putative laccase systems with multiple chemical mediator compounds in high throughput assays to determine optimized systems for PFAS treatment. Aim 2 focuses on studying the reactions of anaerobic radical systems, such as glycyl radical enzymes (GRE) and S-adenosylmethionine (SAM) to study their capability to be engineered future remediation strategies. We will combine Project 3 and 4 approaches in Aim 3, where chemical treatment will be used to prime pollutants that make them more amenable to subsequent biological radical treatment, as well as study the microbial community dynamics before and after chemical treatment. The findings of Project 3 could provide a new approach of remediation technologies to remediate highly halogenated emerging and legacy compounds in the environment to protect the environmental health of surrounding communities.