Collaborative Research: Fluorochemical Signatures in Municipal Waste and Landfill Leachate

现在在人类和野生动物以及水生、陆地和大气环境中都检测到氟化学品。碳氟化合物链的独特特性使其在广泛的应用中非常有用，同时还具有抗非生物和生物降解的能力。全氟辛烷磺酸不会被任何已知的自然过程降解。大多数含氟化学品应用于固体表面（如地毯、纺织品、纸张），这些产品通常在垃圾填埋场处理；然而，人们对将含氟化学物质释放到渗滤液中的过程几乎一无所知。在现代垃圾填埋场，渗滤液被输送到污水处理厂；然而，在废水处理过程中，含氟化学品并没有减少。在数千个没有建造渗滤液收集系统的旧的、封闭的垃圾填埋场中，渗滤液经常被释放到地下水中。迫切需要进行研究，以了解垃圾填埋场作为环境中氟化学品的点源所起的作用。假设1认为，垃圾填埋场中的含氟化学品是通过物理浸出和含氟碳固体的厌氧生物降解从垃圾中释放出来的。假设2：地毯、纺织品和纸张是氟化学品的主要来源，氟化学品的特征是？垃圾可以用来区分垃圾填埋与其他地表水的输入，如城市污水。假设3是垃圾填埋场是含氟化学品的长期来源，是我们国家的重要组成部分？S氟化库存。控制实验室实验，现场抽样和模型将用于评估我们的假设。目标1是量化通过浸出和生物降解从垃圾和垃圾成分中释放的含氟化学品的浓度和组成。实验将在可控的垃圾填埋场模拟反应器中进行，在非生物和生物活性厌氧条件下进行。将获得关于个别含氟化学品和形成无终点、持久性氟化学品形式（包括全氟辛烷磺酸和全氟辛烷磺酸）的总可氧化前体的定量数据。这些数据将用于确定释放个别含氟化学品及其前体的垃圾类型，并使我们能够使含氟化学品的特征合理化。渗滤液。目的2是表征渗滤液中氟化学物质的浓度。将分析美国垃圾填埋场代表性横截面的渗滤液，以评估垃圾年龄、气候和垃圾填埋场运营策略的影响。目标3是利用本研究开发的清单模型，估计在全国范围内排放到工程（如废水处理厂）和自然（如地下水）系统中的氟化学品的质量。智力价值：这一建议是对垃圾填埋场内发生的导致氟化学品释放的过程以及固体废物作为氟化学品来源的相对重要性进行定量评估的第一次努力。该项目将(1)量化导致垃圾填埋场渗滤液中含氟化学品的过程，(2)确定释放含氟化学品的城市垃圾成分，以及(3)为量化垃圾填埋场成为释放到工程和天然水生系统的氟化学品的长期储存库和点源的程度奠定基础。就更广泛的影响而言，这项研究将引起公众的共鸣，因为公众越来越意识到消费品和环境中的微量有机化学物质。pi将利用这种意识，开发一个广为宣传的网站，将快餐外卖盒和抗污纺织品等日常用品与环境工程和化学联系起来。拟议中的研究将允许每所大学的一名博士生参与一个涉及两所大学合作的备受瞩目的项目。清单模型将提供对氟化学品向环境释放的估计，以及探索这一估计中的不确定性的手段，这将对必须优先考虑氟化学品控制工作的监管机构有用。清单模型也将有助于在获得数据后评估来自垃圾填埋场的其他排放，并将作为在全球推广这项工作的起点。

Collaborative Proposal 1067144 PI Field/1066769 PI BarlazFluorochemicals are now detected in both humans and wildlife, as well as in aquatic, terrestrial, and atmospheric environments. The unique characteristics of fluorocarbon chains make them useful in a wide range of applications yet resistant to abiotic and biological degradation. Perfluorooctane sulfonate (PFOS) is not degraded by any known natural processes. The majority of fluorochemicals are applied to solid surfaces (e.g., carpets, textiles, paper) and these products are typically disposed of in landfills; however, virtually nothing is known about the processes that release fluorochemicals into leachate. In modern landfills, leachate is routed to wastewater treatment plants; however, fluorochemicals are not attenuated during wastewater treatment. For the thousands of older, closed landfills that were constructed without leachate collection systems, leachate is often released to groundwater. Research is critically needed to understand the role that landfills play as point sources of fluorochemicals in the environment.Hypothesis 1 is that fluorochemicals in landfills are released from refuse by physical leaching and by anaerobic biodegradation of the fluorocarbon-containing solids. Hypothesis 2 is that carpet, textiles, and paper are the primary sources of fluorochemicals and that the fluorochemical ?signature? of refuse can be used to differentiate landfills from other inputs to surface water such as municipal wastewater effluent. Hypothesis 3 is that landfills represent a long-term source of fluorochemicals and are a significant component of our nation?s fluorochemical inventory. Controlled laboratory experiments, field sampling and a model will be used to assess our hypotheses. Objective 1 is to quantify the concentration and composition of fluorochemicals released from refuse and refuse components by leaching and biodegradation of these refuse components. Experiments will be conducted in controlled landfill simulation reactors under both abiotic and biologically active anaerobic conditions. Quantitative data on individual fluorochemicals and the total oxidizable precursors that form dead-end, persistent fluorochemical forms including PFOS and PFOA will be obtained. The data will be used to identify the types of refuse that release individual fluorochemicals and their precursors and enable us to rationalize the fluorochemical ?signatures? of leachates. Objective 2 is to characterize fluorochemical concentrations in leachate. Leachates from a representative cross section of U.S. landfills will be analyzed to assess the effects of refuse age, climate, and landfill operating strategy. Objective 3 is to estimate the mass of fluorochemicals released to engineered (e.g., wastewater treatment plants) and natural (e.g., groundwater) systems on a national scale using an inventory model developed in this research.Intellectual Merit: This proposal represents the first effort to quantitatively evaluate the processes occurring within landfills that result in fluorochemical release and the relative importance of solid waste as a source of fluorochemicals. This project will (1) quantify the processes that result in fluorochemicals in landfill leachate, (2) establish the components of municipal refuse that release fluorochemicals, and (3) establish the basis for quantifying the degree to which landfills are long-term repositories and point sources of fluorochemicals released to engineered and natural aquatic systems. In terms of the broader impacts, this research will resonate with a public that is increasingly aware of trace organic chemicals in consumer products and in the environment. The PIs will capitalize on this awareness by developing a well-publicized web site that relates everyday items such as fast-food take-out boxes and stain resistant textiles to environmental engineering and chemistry. The proposed research will allow one Ph.D. student at each institution to participate in a high-profile project that involves collaboration between two universities. The inventory model will provide an estimate of fluorochemical release to the environment as well as a means for exploring uncertainty in this estimate that will be useful for regulators who must prioritize fluorochemical control efforts. The inventory model will also be useful for the assessment of other releases from landfills as data become available and will serve as a starting point for extension of this work globally.