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

项目总结/摘要 卤化污染物的生物修复存在挑战，包括供体利用效率低， 缓慢的脱卤，低的脱卤活性和程度， 同时处理共污染物的难度也很大。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的进展，并提出了一个 协同材料-微生物界面，可以实现更快、更深和耐空气的还原 脱卤本文将对电驱动材料-微生物复合体的电荷转移机理进行研究。 这将指导新型纳米和微米尺度材料的设计和优化，以提高 传质效率和加速脱卤。局域电子施主能级可以稳定地 保持在低水平，有利于脱卤呼吸微生物超过产甲烷菌和同型产乙酸菌， 导致增强的电子供体利用。对微生物的系统级理解， 生物电化学系统和基因/酶负责更深层次的去极化将获得与组学 技术.微生物间新的还原性脱氢产物/途径和协同作用 和电化学去离子将阐明使用先进的分析工具，如高分辨率 质谱分析法来此外，用于还原脱卤的耐空气材料-微生物框架将 使用最近设计的微丝阵列电极开发，并实施以实现同时 在开放系统中氧化共污染物1，4-二氧六环。该项目将大大推动 对协同材料中加速和更深层次的还原脱卤的机理理解- 微生物界面这种混合框架由可持续太阳能产生的电力供电 并且可以通过减少可发酵有机物的需求和通过将 厌氧和好氧修复工艺。这种新模式的成功示范， 生物修复将潜在地导致未来用于清除卤化污染物和共 地下环境中的污染物。发达的材料-微生物框架也高度 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.