Enzymatic Biocatalysis of Endocrine Disrupting Chemicals in Wastewater: A Sustainable Technology for Emerging Contaminants

1236730(布伦南)。随着有益的水再利用成为世界各地的普遍做法，人们对残留污染物对水生生态系统和人类健康的影响的担忧正在升级。内分泌干扰物(EDCs)存在于增塑剂、药品、杀虫剂和阻燃剂等日常商业物品中，已被证明可扰乱暴露在其中的生物体的激素功能，即使在非常低的浓度下也会造成不利的生理影响。通常，这些污染物在常规废水处理过程中不会被完全去除，并被排放到接收水中，在那里它们可能会损害生态系统并重新进入饮用水供应。虽然存在一些物理和化学处理方法来处理废水中的EDCs，但这些方法昂贵，而且对世界上大多数国家来说是无法实现的。为了从废水中去除这些新出现的污染物，迫切需要一种廉价、可持续的处理方法。智力上的功绩。这项研究的总体目标是严格评估使用真菌和细菌共生联盟来加强废水处理厂(WWTP)中EDC去除的技术和经济可行性，这些真菌和细菌具有催化消除EDC的能力。尽管真菌已经证明了在含有营养丰富的生长介质的间歇系统中降解内毒素的能力，但在连续流系统中使用菌丝体处理废水中的内毒素的报道还没有报道。然而，PI最近表明，某些真菌能够在废水中生长，并产生能够催化破坏内皮细胞的生物催化酶。同样，最近也有其他研究表明，氨氧化细菌(AOB)可以利用单加氧酶协同代谢降解废水中的某些类污染物，并且在某些情况下，细菌和真菌的相互作用可以导致整体降解能力的协同增强。因此，为了充分发挥污水处理厂生态学的潜力，本研究将结合分析化学和分子微生物学技术，了解污水处理厂中AOB和真菌群落的增强和扩大程度，以及接种和/或自然真菌与AOB之间的协同作用的机理。可以预见，通过促进独特的、酶驱动的生物催化途径，废水处理过程可以优化，以便有效地进行EDC处理，同时最大限度地提高成本效益。为了实现这一目标，一系列批次和生物反应器实验产生的数据将被纳入该技术的生命周期评估(LCA)，以确定其与更传统的物理和化学处理方法相比的相对可持续性。将实验室规模的研究结果与生命周期评估的结果相结合，将能够在中试规模的生态废水处理系统(也称为生态机器)上指导部署EDCs处理技术。如果在试点规模上得到验证，那么其他生态机器系统可以进行类似的转换，传统的废水处理厂可以得到加强或升级，以包括EDC处理。更广泛的影响。除了支持研究生和本科生的研究外，该项目还将通过一个关于安全用水做法的互动网站和生态机器设施的导游向当地社区传播信息。这项工作中开发的技术将是第一次研究酶介导的概念，使用固定化整个菌丝体与AOB相结合来破坏废水中的新污染物，这将比传统的处理方法节省大量的成本。此外，预计将在这项工作期间改进内源性碳化物及其代谢物的分析鉴定和量化，从而能够在了解内源性碳化物的降解途径方面取得进展，从而提高优化处理程序以去除内源性碳化物的能力。最后，LCA驱动的拟议技术开发将提供环境成本和收益的详细核算，并提供一个框架，用于对该过程的经济可行性和长期可行性进行批判性评估，同时提供关于如何改进其设计以获得更大可持续性的见解。这种以系统为基础的方法是全面废水处理的新范例，可作为未来可持续基础设施发展的模式。

1236730 (Brennan). As beneficial water reuse becomes a common practice throughout the world, concern over the effects of residual contaminants on aquatic ecosystems and human health is escalating. Found in everyday commercial items like plasticizers, pharmaceuticals, pesticides, and flame retardants, endocrinedisrupting chemicals (EDCs) have been shown to disrupt hormone function in exposed organisms, causing adverse physiological effects even at very low concentrations. Typically, these contaminants are not completely removed during conventional wastewater treatment, and are discharged into receiving waters where they can potentially harm ecosystems and re-enter potable water supplies. Although some physical and chemical treatment methods exist for treating EDCs in wastewater, they are expensive and unattainable for the majority of the world. An inexpensive, sustainable treatment method is sorely needed for removing these emerging contaminants from wastewater. Intellectual Merit. The overall objective of this research is to critically evaluate the technical and economic feasibility of enhancing EDC removal in wastewater treatment plants (WWTPs) using a symbiotic consortium of fungi and bacteria with a demonstrated ability to catalyze the elimination of EDCs. Although fungi havedemonstrated such a capacity to degrade EDCs in batch systems containing nutrient-rich growth media, the use of mycelia in continuous-flow systems for the treatment EDCs in wastewater has not been reported. The PI has recently shown, however, that certain fungi are able to grow in wastewater and produce biocatalytic enzymes that are capable of catalyzing the destruction of EDCs. Similarly, others have recently shown that ammonia oxidizing bacteria (AOB) can co-metabolically degrade certain classes of contaminants in wastewater using monoxygenase enzymes, and that in certain scenarios, bacteria-fungi interactions can result in a synergistic enhancement of overall degradative capacity. Therefore, to realize the full potential of WWTP ecology, this research will combine analytical chemistry and molecular microbiology techniques to understand the extent to which the AOB and fungal communities can be enhanced and augmented, and the mechanisms by which synergism can be promoted between inoculated and/or native fungi and AOB in WWTPs. It is envisioned that by promoting unique, enzyme-drivenbiocatalytic pathways, wastewater treatment processes can be optimized for effective EDC treatment while maximizing cost effectiveness. To meet this objective, data generated from a series of batch and bioreactor experiments will be incorporated into a Life Cycle Assessment (LCA) of the technology to determine its relative sustainability compared to more conventional physical and chemical treatment methods. Combining the results of lab-scale research with LCA results will enable a guided deployment of the technology for the treatment of EDCs at a pilot-scale ecological wastewater treatment system (a.k.a., eco-machine). If validated at the pilot-scale, then other eco-machine systems could be similarly converted, and conventional wastewater treatment plants could be enhanced or upgraded to include EDC-treatment. Broader Impact. In addition to supporting graduate and undergraduate student research, this project will disseminate information to the local community through an interactive website on safe water practices and guided tours of an eco-machine facility. The technology developed in this work would be the first to investigate the concept of enzyme-mediated destruction of emerging contaminants in wastewater using immobilized whole mycelia in combination with AOB, which could represent a significant cost savings over traditional treatment methods. Additionally, it is expected that improvements in the analytical identification and quantification of EDCs and their metabolites will be developed during this work, enabling progress in the understanding of EDC-degradation pathways, and thereby increasing the ability to optimize treatment processes for their removal. Finally, the LCA-driven development of the proposed technology will provide a detailed accounting of environmental costs and benefits and provide a framework for critical evaluation of the economic feasibility and long-term viability of the process, while providing insight into how its design can be improved for greater sustainability. This systems-based approach is a new paradigm for holistic wastewater treatment, which could serve as a model for the future development of sustainable infrastructure.