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

该奖项由化学学部环境化学科学（ECS）项目资助。它是由加州大学河滨分校的刘金勇教授和David Volz教授以及伊利诺伊大学厄巴纳-香槟分校的Yujie Men教授合作完成的。他们与研究生一起研究全氟化合物（pfc）。全氟化合物是一类化学物质，与碳氢化合物具有相同的碳主链，但与碳主链相连的所有原子都是氟而不是氢。碳氟键是高度稳定的。用pfc改性的表面既耐水又耐油。因此，全氟化合物广泛应用于消防泡沫、电子产品、润滑剂、户外服装和设备以及不粘炊具中。C-F键的稳定性使得pfc在自然环境中也很难降解。合成全氟化合物已在全球环境和生物体中被检测到。全氟化合物的生物积累与各种人类健康问题有关。然而，目前的技术还不能有效地通过破坏C-F键来降解PFC（即去氟化）。因此，需要开发更容易降解的新型全氟化合物和从环境中去除这些化合物的新策略。本研究探讨了在非生物和微生物环境下，钴催化PFCs脱除氟的构效关系、反应机理和产物。研究结果可能有助于解决PFC污染挑战，为设计新型可降解PFC和自然环境中的微生物修复提供基本指导。本研究采用多方面的方法，结合化学和生物工具来研究钴（Co）催化全氟化合物的脱氟。研究小组研究了共催化反应后PFC脱氟的产物。研究了化学和生物合成配合物中Co配位球与脱氟活性的构效关系。确定了非生物和微生物除氟反应的氧化还原环境。3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。广泛的社区是通过面向公众的科学会议和其他活动达成的。研究结果可应用于仿生催化剂体系的设计、新型含氟药物的合成以及新型含氟化学品的毒理学评价。该项目的成果对工业氟化设计的转变具有广泛的影响。研究工作与教育和推广计划相结合，旨在扩大代表性不足的少数民族在化学、环境科学和化学/环境工程方面的参与。

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.