Model-aided Design and Integration of Functionalized Hybrid Nanomaterials for Enhanced Bioremediation of Per-and Polyfluoroalkyl Substances (PFASs)

功能化杂化纳米材料的模型辅助设计和集成，用于增强全氟烷基物质和多氟烷基物质 (PFAS) 的生物修复

• 批准号: 10319174
• 负责人: Diana S Aga
• 金额: $ 30.99万
• 依托单位: STATE UNIVERSITY OF NEW YORK AT BUFFALO
• 依托单位国家: 美国
• 财政年份: 2021
• 资助国家: 美国
• 起止时间: 2021-01-01 至 2025-10-31
• 项目状态: 未结题
• 来源: https://reporter.nih.gov/project-details/10319174
• 关键词: Acids; Aftercare; Amino Acids; Anaerobic Bacteria; Bacteria; Binding; Biodegradation; Biological; Bioremediations; Blood; Carbon; Characteristics; Chemicals; Chromatography; Communities; Couples; Degradation Pathway; Development; Docking; Environment; Environmental Pollution; Enzyme Interaction; Enzymes; Equilibrium; Evolution; Excision; Exposure to; Fluorine; Genes; Genetic Transcription; Goals; Hazardous Chemicals; Head; Health; Human; Hybrids; Hydrogen Peroxide; Industrialization; Ions; Iron; Kidney; Kinetics; Knowledge; Length; Link; Liquid Chromatography; Malignant Neoplasms; Malignant neoplasm of liver; Mass Spectrum Analysis; Measurable; Measures; Metagenomics; Metals; Microbiology; Minerals; Modeling; Molecular; NMR Spectroscopy; Nanotechnology; Non-Insulin-Dependent Diabetes Mellitus; Outcome; Oxidation-Reduction; Oxides; Pathway interactions; Persons; Plants; Poison; Poly-fluoroalkyl substances; Production; Property; Public Health; Reaction; Research; Resolution; Risk; Site; Site-Directed Mutagenesis; Source; Structure; Surface; System; Techniques; Technology; Testing; Toxic effect; Toxicokinetics; Training; Treatment Step; Validation; Work; catalyst; consumer product; dehalogenation; design; drinking water; efficacy testing; exposed human population; graphene; ground water; improved; in silico; innovation; insight; liver injury; metallicity; microbial; microbial community; microbial genome; microbiota; microorganism; mineralization; molecular dynamics; molecular modeling; nano; nanomaterials; novel; oxidation; prevent; rRNA Genes; remediation; titanium dioxide; tool; transcriptomics; ultraviolet irradiation

PROJECT SUMMARY Environmental contamination by per- and polyfluoroalkyl substances (PFASs) is a major public health concern because of the wide range of toxic effects that have been associated with exposure to these persistent chemicals. Due to the strong stability of the C-F bond, very few microorganisms have been found capable of degrading PFASs, and the biodegradation is very slow and incomplete. Often, bioremediation efforts result in the formation of shorter chain PFASs that remain toxic, persistent, and highly mobile in the environment. Current abiotic treatment technologies can be more effective, but have very high energy requirements. Therefore, this research proposes an innovative remediation strategy that couples a pre-treatment step using catalytic hybrid nanomaterials with biodegradation using enriched microbial communities to achieve more efficient and complete destruction of PFASs without the formation of toxic by-products. Multifunctional reduced graphene oxide-metallic nanohybrids (e.g. rGO-nZVI-TiO2) that are capable of catalyzing defluorination and oxidation of PFASs will be synthesized and characterized for their efficiencies in converting highly stable PFASs to more biodegradable forms. Pure cultures (e.g. Dehalococcoides sp. and Dehalobacter sp.) and enriched microbial consortia collected from PFAS-contaminated sites and anaerobic wastewater treatment plants will be used to degrade different types of PFASs and measure their removal efficacy. Using metagenomic and transcriptomic tools, the microorganisms responsible for degradation, their functional characteristics, and the genes being transcribed during defluorination will be identified. By-products formed at each step of the pre-treatment reaction, and during the course of the microbial degradation of PFASs will be characterized using liquid chromatography with high- resolution mass spectrometry, 19F-nuclear magnetic resonance spectroscopy, and ion chromatography to obtain information on the identities of PFASs transformation products, degradation kinetics, and mass balance. Molecular modeling will be used to bring mechanistic insight into specific PFAS-surface and PFAS-enzyme interactions. The effect of the structural features of PFASs (i.e. branching, chain-length, type of head groups) on their biodegradability will be systematically evaluated, first by molecular modeling, and then by experimental validation. Knowledge from the chemical characterization of PFASs degradation by-products combined with in silico site-directed mutagenesis will facilitate the tuning of enzymatic activities and discovery of novel bacteria that are efficient degraders of PFASs from the natural environment. These insights will guide the systematic design of highly efficient nano-enhanced bioremediation systems for complete microbial degradation of PFASs.

项目摘要 全氟烷基和多氟烷基物质（PFASs）造成的环境污染是一个重大的公共卫生问题 因为接触这些持久性化学品会产生广泛的毒性效应。 由于C-F键的强稳定性，很少有微生物被发现能够降解 PFASs，生物降解非常缓慢和不完全。通常，生物修复的努力导致形成 短链PFASs在环境中保持毒性、持久性和高度移动的。当前非生物 处理技术可以更有效，但需要非常高的能源。因此本研究 提出了一种创新的补救策略，耦合预处理步骤，使用催化混合 纳米材料与生物降解利用丰富的微生物群落，以实现更有效和完整的 销毁PFASs而不形成有毒副产品。多功能还原氧化石墨烯-金属 能够催化PFAS脱附和氧化的纳米杂化物（例如rGO-nZVI-TiO 2）将被 合成并表征了它们将高度稳定的PFAS转化为更可生物降解的PFAS的效率 forms.纯培养物（如Dehalococcoides sp.和Dehalococcus sp.）并收集了丰富的微生物群落 从PFAS污染的场地和厌氧废水处理厂将用于降解不同的 PFASs的类型，并测量其去除效果。使用宏基因组学和转录组学工具， 负责降解的微生物、其功能特征和转录的基因 将被识别。在预处理反应的每个步骤中形成的副产物，以及在预处理过程中形成的副产物。 PFASs的微生物降解过程将采用液相色谱法进行表征， 分辨率质谱法、19 F-核磁共振光谱法和离子色谱法，以获得 关于PFASs转化产物的特性、降解动力学和质量平衡的信息。 分子模拟将被用来使机制洞察特定的PFAS-表面和PFAS-酶 交互. PFAS的结构特征（即支化、链长、头基类型）对 它们的生物降解性将被系统地评估，首先通过分子建模，然后通过实验 验证。从PFASs降解副产物的化学表征中获得的知识， 计算机定点诱变将有助于酶活性的调整和新细菌的发现 它们是自然环境中PFASs的高效降解剂。这些见解将指导系统的 设计高效的纳米强化生物修复系统，以完全微生物降解PFASs。