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: 1930959
• 负责人: Paschalis Alexandridis
• 金额: $ 28.22万
• 依托单位: SUNY at Buffalo
• 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 2024-08-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1930959&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.

表面活性剂是含有水不溶的（或油溶性）成分和水溶性成分的分子。 由于具有该特性，因此在多种应用中使用表面活性剂，例如洗涤剂，乳化剂，泡沫剂和分散剂。 氟化的表面活性剂发现了各种各样的工业和消费者应用，因为它们具有较高的化学和热稳定性及其独特的能力，可以使表面像特氟龙一样，并且与水和碳氢化合物都不混乱。 由于其稳定性，氟化的表面活性剂也可能极大地抵抗环境中的降解，生物弥补并引起不利的健康影响。 由于环境中的毒性和持久性，两种氟化的表面活性剂（PFOA）和全氟辛烷磺酸盐（PFO）已在美国逐步消失。 正在引入几种新的氟化表面活性剂，其中很少有关于其性质的信息。 该协作研究项目结合了实验和计算方法，以研究水溶液中氟化表面活性剂的分子组织。 这些研究将着重于量化这种新兴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理解来从水生环境和生物群中去除氟化的表面活性剂。该研究项目有三个目标：（1）通过使用协调的实验表征和分子建模工作来了解水溶液中定义明确的氟化表面活性剂的纳米级组织。 重点是提高计算能力以预测和匹配实验结果； （2）建立并量化负责氟化表面活性剂分子组织的关键驱动力，并与其他化合物（聚合物，脂质，环糊精，环糊精）相互作用，并存在于水溶液和液体/固体界面中。 重点是新兴的氟化表面活性剂以及与环境和健康问题有关的相互作用； （3）设计和开发用于物理过程中的材料，以捕获氟化表面活性剂及其从水性介质中取出。预测分子组织和氟化表面活性剂的相互作用以及相应的结构性质关系的能力可以使新材料和方法的合理设计用于分离氟化表面活性剂。 这项研究的结果应允许对新的化学设计的核对层评估，以替代配方和产品中氟化分子的潜在替代。该研究项目是研究生进行尖端研究的培训理由。 研究人员还将吸引本科生参与研究，并将该项目与外展和课程发展活动相结合。该奖项反映了NSF的法定任务，并使用基金会的知识分子优点和更广泛的审查标准，认为值得通过评估来获得支持。

项目成果

Perfluorooctanoate in Aqueous Urea Solutions: Micelle Formation, Structure, and Microenvironment

• DOI: 10.3390/ijms20225761
• 发表时间: 2019-11-01
• 期刊: INTERNATIONAL JOURNAL OF MOLECULAR SCIENCES
• 影响因子: 5.6
• 作者: Kancharla, Samhitha;Canales, Emmanuel;Alexandridis, Paschalis
• 通讯作者: Alexandridis, Paschalis

Controlling the self-assembly of perfluorinated surfactants in aqueous environments

• DOI: 10.1039/d1cp00049g
• 发表时间: 2021-04-14
• 期刊: PHYSICAL CHEMISTRY CHEMICAL PHYSICS
• 影响因子: 3.3
• 作者: Dong, Dengpan;Kancharla, Samhitha;Alexandridis, Paschalis
• 通讯作者: Alexandridis, Paschalis

Association between Nonionic Amphiphilic Polymer and Ionic Surfactant in Aqueous Solutions: Effect of Polymer Hydrophobicity and Micellization

• DOI: 10.3390/polym12081831
• 发表时间: 2020-08-01
• 期刊: POLYMERS
• 影响因子: 5
• 作者: Kancharla, Samhitha;Zoyhofski, Nathan A.;Alexandridis, Paschalis
• 通讯作者: Alexandridis, Paschalis

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

Structure and Interactions in Perfluorooctanoate Micellar Solutions Revealed by Small-Angle Neutron Scattering and Molecular Dynamics Simulations Studies: Effect of Urea

小角中子散射和分子动力学模拟研究揭示全氟辛酸酯胶束溶液的结构和相互作用：尿素的影响

• DOI: 10.1021/acs.langmuir.1c00433
• 发表时间: 2021
• 期刊: Langmuir
• 影响因子: 3.9
• 作者: Kancharla, Samhitha;Dong, Dengpan;Bedrov, Dmitry;Tsianou, Marina;Alexandridis, Paschalis
• 通讯作者: Alexandridis, Paschalis