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SusChEM: Collaborative Research: Cobalt-catalyzed Defluorination of Branched Perfluorinated Compounds

SusChEM：合作研究：钴催化支链全氟化合物脱氟

基本信息

批准号：
1709286
负责人：
Wen-Tso Liu
金额：
$ 21.63万
依托单位：
University of Illinois at Urbana-Champaign
依托单位国家：
美国
项目类别：
Standard Grant
财政年份：
2017
资助国家：
美国
起止时间：
2017-09-01 至 2020-08-31
项目状态：
已结题

来源：
https://www.nsf.gov/awardsearch/showAward?AWD_ID=1709286&HistoricalAwards=false
关键词：
SusChEM Collaborative Research Cobalt catalyzed

项目摘要

This award is funded by the Environmental Chemical Sciences (ECS) Program in the Division of Chemistry. It is a collaboration between Professors Jinyong Liu and David Volz at the University of California, Riverside, and Prof. Yujie Men at the University of Illinois at Urbana-Champaign. Together with their graduate students they study perfluorinated compounds (PFCs). PFCs are a family of chemicals that have the same carbon backbone as hydrocarbons but all atoms attached to the carbon backbone are fluorine instead of hydrogen. Carbon-fluorine (C-F) bonds are highly stable. Surfaces modified with PFCs are resistant to both water and oil. Thus, PFCs are widely used in fire-fighting foams, electronics, lubricants, outdoor apparel and equipment, and on-sticking cooking ware. The stability of C-F bonds makes PFCs also very difficult to degrade in the natural environment. Synthetic PFCs have been globally detected in the environment and living organisms. Bioaccumulation of PFCs has been connected to a variety of human health problems. However, current technologies are not effective in PFC degradation via breaking the C-F bonds (i.e., defluorination). Therefore, it is desired to develop both new PFCs that can be degraded more easily and new strategies for removing these compounds from the environment. This research investigates the structure-activity relationships, reaction mechanisms, and products of cobalt-catalyzed removal of fluorine from of PFCs in abiotic and microbial environments. Outcomes may contribute to solving PFC pollution challenges by providing fundamental guidelines to the design of novel degradable PFCs and microbial remediation in natural environments.This research employs a multi-faceted approach combining chemical and biological tools to investigate cobalt (Co)-catalyzed defluorination of PFCs. The team investigates the product of PFC defluorination after Co-catalyzed reactions. The structure-activity relationship between the Co coordination sphere in chemically and biologically synthesized complexes and the defluorination activity is investigated. The redox environment enabling abiotic and microbial defluorination reactions is determined. Three PhD students receive interdisciplinary training. Undergraduate and high school researchers from a diverse student population are exposed to interdisciplinary training, specifically topics related of sustainability. The broad community is reached via a public-oriented science conference and other events. Results may be applied to biomimetic catalyst system design, synthesis of novel fluoro-pharmaceuticals, and toxicology evaluation of novel fluorochemicals. Outcomes of this project have broad impacts on transforming industrial fluorochemical design. Research efforts are coupled with educational and outreach plans designed to broaden participation from underrepresented minorities in Chemistry, Environmental Science, and Chemical / Environmental Engineering.

该奖项由化学部的环境化学科学（ECS）计划资助。这是滨江的加州大学的刘金勇教授和大卫沃尔兹教授与伊利诺伊大学厄巴纳-香槟分校的门宇杰教授的合作。他们与研究生一起研究全氟化合物（PFC）。PFC是一种化学物质家族，具有与碳氢化合物相同的碳骨架，但连接到碳骨架上的所有原子都是氟而不是氢。碳-氟（C-F）键是高度稳定的。用PFC改性的表面既防水又耐油。因此，全氟化碳被广泛用于灭火泡沫、电子产品、润滑剂、户外服装和设备以及粘附式炊具。C-F键的稳定性使得PFCs在自然环境中也很难降解。在全球环境和生物体中都检测到了合成全氟化碳。全氟化学品的生物累积与各种人类健康问题有关。然而，目前的技术在通过破坏C-F键（即，延迟）。因此，需要开发可以更容易降解的新的PFC和从环境中去除这些化合物的新策略。本研究探讨了钴催化去除非生物和微生物环境中全氟碳化物中氟的构效关系、反应机理和产物。本研究采用化学和生物相结合的方法研究了钴催化降解PFCs的反应机理，为新型可降解PFCs的设计和自然环境中的微生物修复提供了基础指导，为解决PFCs污染问题提供了理论依据。该团队研究了在Co催化反应后PFC脱氟的产物。研究了化学合成和生物合成配合物中钴配位球与其脱氯活性之间的构效关系。确定了使非生物和微生物脱硫反应的氧化还原环境。三名博士生接受跨学科培训。来自不同学生群体的本科和高中研究人员接受跨学科培训，特别是与可持续发展相关的主题。广泛的社区通过面向公众的科学会议和其他活动达到。研究结果可应用于仿生催化剂体系设计、新型含氟药物的合成以及新型含氟化合物的毒理学评价。该项目的成果对改变工业氟化学品设计具有广泛的影响。研究工作与教育和推广计划相结合，旨在扩大在化学，环境科学和化学/环境工程中代表性不足的少数民族的参与。