Collaborative Research: Fluorinated Surfactants: Molecular Organization and Binding in Solution and on Surfaces

合作研究：氟化表面活性剂：溶液和表面上的分子组织和结合

• 批准号: 1930935
• 负责人: Dmitry Bedrov
• 金额: $ 18.09万
• 依托单位: University of Utah
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2019
• 资助国家: 美国
• 起止时间: 2019-09-01 至 2022-08-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1930935&HistoricalAwards=false
• 关键词: Collaborative; Research; Fluorinated; Surfactants; Molecular

Surfactants are molecules that contain both a water-insoluble (or oil-soluble) component and a water-soluble component. Because of this property, surfactants are used in a wide range of applications such as detergents, emulsifiers, foaming agents, and dispersants. Fluorinated surfactants find a wide variety of industrial and consumer applications because of their high chemical and thermal stability and their unique abilities to render surfaces Teflon-like and to be immiscible with both water and hydrocarbons. Due to their stability, fluorinated surfactants also can be extremely resistant to degradation in the environment, bioaccumulate, and cause adverse health effects. Two fluorinated surfactants, perfluorooctanoic acid (PFOA) and perfluorooctane sulfonate (PFOS), have been phased out in the U.S. due to their toxicity and persistence in the environment. Several new fluorinated surfactants are being introduced for which very little information is available in the open literature about their properties. This collaborative research project combines experimental and computational methods to study the molecular organization of fluorinated surfactants in aqueous solutions. The studies will focus on quantifying how such emerging surfactants bind to other molecules or surfaces and how a fundamental understanding of such interactions can be utilized for the removal of fluorinated surfactants from the aquatic environment and biota. This research project has three objectives: (1) To understand nanoscale organization of well-defined fluorinated surfactants in aqueous solutions by using coordinated experimental characterization and molecular modeling efforts. The focus is on advancing computational capabilities to predict and match experimental results; (2) To establish and quantify key driving forces responsible for fluorinated surfactant molecular organization and interactions with other compounds (polymers, lipids, cyclodextrins) present in aqueous solutions and at liquid/solid interfaces. The focus is on emerging fluorinated surfactants and on interactions that are relevant to environmental and health concerns; and (3) To design and develop materials used in physical processes for the capture of fluorinated surfactants and their removal from aqueous media. The ability to predict molecular organization and interactions of fluorinated surfactants, and corresponding structure property relationships, can enable the rational design of new materials and methods for separating fluorinated surfactants. The results of this research should permit the in-silico evaluation of new chemical designs for potential replacements of fluorinated molecules in formulations and products. The research project serves as a training ground for graduate students to perform cutting edge research. The researchers also will engage undergraduate students in research and integrate the project with outreach and curriculum development activities.This award reflects NSF's statutory mission and has been deemed worthy of support through evaluation using the Foundation's intellectual merit and broader impacts review criteria.

表面活性剂是既含有不溶于水的(或油溶的)成分又含有可溶于水的成分的分子。由于这一特性，表面活性剂被广泛应用于洗涤剂、乳化剂、发泡剂和分散剂等。含氟表面活性剂因其高度的化学和热稳定性以及独特的表面处理能力而被广泛应用于工业和消费领域，这些表面活性剂可以使表面呈特氟龙状，并与水和碳氢化合物不相容。由于其稳定性，含氟表面活性剂还可以极大地抵抗环境中的降解，生物积累，并造成不利的健康影响。全氟辛酸(PFOA)和全氟辛烷磺酸(PFOS)这两种含氟表面活性剂因其在环境中的毒性和持久性，在美国已被逐步淘汰。几种新的氟化表面活性剂正在被引入，关于它们的性质的公开文献中关于它们的信息很少。这一合作研究项目结合了实验和计算方法来研究含氟表面活性剂在水溶液中的分子组织。这些研究将侧重于量化这些新出现的表面活性剂如何与其他分子或表面结合，以及如何利用对这种相互作用的基本了解来从水环境和生物群中去除含氟表面活性剂。本研究项目有三个目标：(1)通过协调的实验表征和分子模拟工作，了解明确定义的含氟表面活性剂在水溶液中的纳米级组织。重点是提高预测和匹配实验结果的计算能力；(2)建立和量化导致氟化表面活性剂分子组织以及与存在于水溶液和液/固界面的其他化合物(聚合物、脂类、环糊精)相互作用的关键驱动力。重点是新出现的含氟表面活性剂以及与环境和健康相关的相互作用；以及(3)设计和开发物理过程中用于捕获含氟表面活性剂并将其从水介质中去除的材料。能够预测含氟表面活性剂的分子结构和相互作用，以及相应的结构性质关系，可以合理设计分离含氟表面活性剂的新材料和新方法。这项研究的结果应该允许对配方和产品中潜在的氟分子替代品的新化学设计进行电子计算机评估。该研究项目作为研究生进行尖端研究的训练场。研究人员还将让本科生参与研究，并将该项目与外展和课程开发活动相结合。该奖项反映了NSF的法定使命，并通过使用基金会的智力优势和更广泛的影响审查标准进行评估，被认为值得支持。

项目成果

Adsorption Mechanism of Perfluorooctanoate on Cyclodextrin-Based Polymers: Probing the Synergy of Electrostatic and Hydrophobic Interactions with Molecular Dynamics Simulations

• DOI: 10.1021/acsmaterialslett.2c00168
• 发表时间: 2022-05-02
• 期刊: ACS MATERIALS LETTERS
• 影响因子: 11.4
• 作者: Choudhary, Aditya;Dong, Dengpan;Bedrov, Dmitry
• 通讯作者: Bedrov, Dmitry

Binding of Perfluorooctanoate to Poly(ethylene oxide)

全氟辛酸酯与聚环氧乙烷的结合

• DOI: 10.1021/acs.macromol.2c00371
• 发表时间: 2022
• 期刊: Macromolecules
• 影响因子: 5.5
• 作者: Kancharla, Samhitha;Dong, Dengpan;Bedrov, Dmitry;Alexandridis, Paschalis;Tsianou, Marina
• 通讯作者: Tsianou, Marina

Structure and composition of mixed micelles formed by nonionic block copolymers and ionic surfactants in water determined by small-angle neutron scattering with contrast variation

• DOI: 10.1016/j.jcis.2021.10.176
• 发表时间: 2022-03-01
• 期刊: JOURNAL OF COLLOID AND INTERFACE SCIENCE
• 影响因子: 9.9
• 作者: Kancharla, Samhitha;Bedrov, Dmitry;Alexandridis, Paschalis
• 通讯作者: Alexandridis, Paschalis

Interaction of Short-Chain PFAS with Polycationic Gels: How Much Fluorination is Necessary for Efficient Adsorption?

• DOI: 10.1021/acsmacrolett.2c00383
• 发表时间: 2022-08
• 期刊: ACS macro letters
• 影响因子: 5.8
• 作者: Aditya Choudhary;D. Bedrov