Synergistic Material-Microbe Interface towards Faster, Deeper, and Air-tolerant Reductive Dehalogenation

项目摘要/摘要 在卤化污染物的生物修复方面存在挑战，包括捐赠者利用效率低和 新出现的全氟和多氟的脱卤剂脱卤率和脱卤度低 物质，以及同时处理共同污染物的困难。为了应对这些挑战， 该项目整合了材料科学和微生物还原脱卤化方面的进展，并提出了一种 协同材料-微生物界面，可实现更快、更深、耐空气的还原 去卤化。提出的电驱动材料-微生物杂化中的电荷转移机制将是 这将指导新型纳米和微米材料的设计和优化，以增强 提高传质效率，加速脱卤化。局域电子给体能级可以稳定地 维持在较低水平，有利于脱卤素呼吸微生物，而不是产甲烷菌和高乙酸菌， 从而提高了电子给体的利用率。对丰富的微生物的系统级理解 生物电化学系统和负责更深层次脱氟的基因/酶将通过组学获得 技巧。新型还原脱氟产物/途径及微生物间的协同作用 电化学除氟将使用先进的分析工具，如高分辨率 质谱学。此外，一种用于还原脱卤化的耐空气材料-微生物框架将 使用最近设计的微线阵列电极进行开发并实现并发 1，4-二恶烷在开放体系中的氧化。这一项目将大大推进 对协同材料中加速深度还原脱卤化的机理理解-- 微生物界面。这一混合框架由可持续太阳能发电提供动力。 并可通过减少对可发酵有机物的需求和通过将 厌氧和好氧修复工艺。这一新范式的成功示范 生物修复可能会导致未来在清除卤代污染物和共污染方面的应用。 地下环境中的污染物。所开发的材料-微生物骨架也高度 可转化为其他环境污染物的生物修复过程。

Project Summary/Abstract Challenges exist in bioremediation of halogenated contaminants, including low donor utilization efficiency and slow dehalogenation, low dehalogenation activity and degree for the emerging per- and polyfluorinated substances, as well as the difficulty in simultaneously treating co-contaminants. To address those challenges, this project integrates advances in materials sciences and microbial reductive dehalogenation and proposes a synergistic materials-microbe interface that can achieve faster, deeper, and air-tolerant reductive dehalogenation. Charge transfer mechanisms in the proposed electricity-driven materials-microbe hybrid will be investigated, which will guide the design and optimization of novel nano- and micro-scale materials to enhance the mass-transport efficiency and accelerate dehalogenation. The local electron donor levels can be stably maintained at low levels, favoring dehalorespiring microorganisms over methanogens and homoacetogens, leading to enhanced electron donor utilization. A systems-level understanding of microorganisms enriched in the bioelectrochemical system and genes/enzymes responsible for deeper defluorination will be obtained with omics techniques. Novel reductive defluorination products/pathways and synergistic interactions between microbial and electrochemical defluorination will be elucidated using advanced analytical tools such as high-resolution mass spectrometry. Furthermore, an air-tolerant materials-microbe framework for reductive dehalogenation will be developed using a recently designed microwire array electrodes and implemented to achieve concurrent oxidation of the co-contaminant 1,4-dioxane in an open system. This project will significantly advance the mechanistic understanding of the accelerated and deeper reductive dehalogenation at the synergistic materials- microbe interface. This hybrid framework is powered by electricity that can be generated from sustainable solar energy and may lower the cost by reducing the requirement of fermentable organics and by combining the anaerobic and aerobic remediation processes. The successful demonstration of this new paradigm of bioremediation will potentially lead to future applications for cleaning up the halogenated contaminants and co- contaminants in subsurface environments. The developed materials-microbe framework is also highly transformable to the bioremediation processes of other environmental contaminants.