Atmospheric Fullerene Chemistry: Elucidating Oxidative Pathways and Characterization of Corresponding Derivatives

大气富勒烯化学：阐明氧化途径和相应衍生物的表征

• 批准号: 1236865
• 负责人: John Fortner
• 金额: $ 30万
• 依托单位: Washington University
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2012
• 资助国家: 美国
• 起止时间: 2012-09-01 至 2015-08-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1236865&HistoricalAwards=false
• 关键词: Atmospheric; Fullerene; Chemistry; Elucidating; Oxidative

NSF 13-1179Environmental Health and Safety of NanotechnologyProgram Manager: Dr. Barbara KarnProposal #1236865Atmospheric Fullerene Chemistry: Elucidating Oxidative Pathways and Characterization of Corresponding DerivativesAbstract: Carbon based nano-scale materials such as fullerenes and nanotubes in particular have been proposed for a variety of applications and are now on track to be widely produced at the industrial scale. Of particular interest, and currently deeply lacking in information/data, is the role of atmospheric processes (e.g. oxidizing reaction scenarios) to significantly alter a wide breadth of fullerene environmental behavior(s) including: solubility, (bio)availability, reactivity, stability, toxicity and overall environmental impact. This project is designed to fundamentally evaluate the reactivity (including kinetic and derivative analyses) of solid state and aqueous available fullerene species under various, highly controlled, atmospheric conditions, focused on oxidation pathways. The overarching hypothesis of this project is that C60, as a model fullerene, can be chemically oxidized and physically altered by a variety of oxidative, yet ubiquitous, processes in the atmosphere. Sub-hypotheses include: (A) Multiple, competing oxidative reactions occur simultaneously, albeit with different kinetics, resulting in corresponding and various derivatives; (B) Under "wet" conditions (10% RH), fullerenes will become increasingly hydrophilic, dissolving aggregates, with hydrolysis as major reaction after initial oxidation; (C) Model (atmospheric) organics and inorganics in the gas phase will modify these kinetics; (D) Reaction products from "wet" reactions (10% RH) will be relatively stable in aqueous systems; whereasunder "dry" reaction conditions, derivatives will continue to react with water upon aqueous exposure.Intellectual Merit: At the conclusion of this project, we will have a vastly improved understanding of environmentally relevant chemical mechanisms/pathways and physico-chemical factors that control the rate and extent of fullerene aggregation, transformation(s) and stabilities under atmospheric conditions. This information will provide fundamental understanding for material life cycle(s) in addition to aiding in the interpretation of fullerene toxicological studies. Results will also provide information regarding fullerene stability, storage and commercial applications, and will contribute to the development of green fullerene chemistries.Broader Impacts: In addition to creating and disseminating new technical knowledge needed for decision-making regarding an industrially produced, engineered nanomaterial; this project (platform) is designed to broadly impact both undergraduate and graduate education and research, in addition to contributing to specific K-12 outreach programs. Graduate and undergraduate(project integrated) education and highly interdisciplinary research will strengthen our human resource base in an emerging need area where qualified researchers are in short supply, yet needed for the development of sustainable nanotechnologies. Furthermore, PI's will support and work directly with educators and students, providing expertise and regular mentoring at the St. Louis' Knowledge is Power Program (KIPP): Inspire Academy, preparing students for local, regional and international science fair projects and competitions.

NSF 13-1179纳米技术环境健康与安全项目经理：Barbara Karn博士提案#1236865大气富勒烯化学：阐明氧化途径和相应衍生物的表征摘要：碳基纳米材料（例如富勒烯和纳米管）已被提议用于各种应用现在有望在工业领域广泛生产 规模。特别令人感兴趣且目前严重缺乏信息/数据的是大气过程（例如氧化反应场景）在显着改变富勒烯环境行为方面的作用，包括：溶解度、（生物）可用性、反应性、稳定性、毒性和总体环境影响。该项目旨在从根本上评估固态和水性可用富勒烯物种在各种高度受控的大气条件下的反应性（包括动力学和导数分析），重点关注氧化途径。该项目的总体假设是，C60 作为一种富勒烯模型，可以通过大气中各种普遍存在的氧化过程进行化学氧化和物理改变。子假设包括： (A) 多个竞争性氧化反应同时发生，尽管动力学不同，产生相应的各种衍生物； (B) 在“湿”条件下（10% RH），富勒烯将变得越来越亲水，溶解聚集体，初始氧化后水解为主要反应； (C) 气相中的模型（大气）有机物和无机物将改变这些动力学； (D) “湿”反应（10% RH）的反应产物在水性体系中相对稳定；而在“干”反应条件下，衍生物在接触水后将继续与水反应。 智力优点：在该项目结束时，我们将对环境相关的化学机制/途径以及控制大气条件下富勒烯聚集、转化和稳定性的速率和程度。除了帮助解释富勒烯毒理学研究之外，这些信息还将提供对材料生命周期的基本了解。结果还将提供有关富勒烯稳定性、储存和商业应用的信息，并将有助于绿色富勒烯化学的发展。 更广泛的影响：除了创造和传播有关工业生产的工程纳米材料决策所需的新技术知识之外；该项目（平台）旨在广泛影响本科生和研究生的教育和研究，此外还为特定的 K-12 外展计划做出贡献。研究生和本科生（项目综合）教育和高度跨学科的研究将加强我们在新兴需求领域的人力资源基础，该领域合格的研究人员短缺，但可持续纳米技术的发展又需要。此外，PI 将支持教育工作者和学生并直接与他们合作，在圣路易斯知识就是力量计划 (KIPP)：Inspire Academy 中提供专业知识和定期指导，帮助学生为当地、区域和国际科学博览会项目和竞赛做好准备。

项目成果

Atmospheric Reactivity of Fullerene (C 60 ) Aerosols

富勒烯 (C 60 ) 气溶胶的大气反应性

• DOI: 10.1021/acsearthspacechem.7b00116
• 发表时间: 2018-02
• 期刊: ACS Earth and Space Chemistry
• 影响因子: 3.4
• 作者: Mitroo, Dhruv;Wu, Jiewei;Colletti, Peter F.;Lee, Seung Soo;Walker, Michael J.;Brune, William H.;Williams, Brent J.;Fortner, John D.
• 通讯作者: Fortner, John D.

Assessing the degree of plug flow in oxidation flow reactors (OFRs): a study on a potential aerosol mass (PAM) reactor

评估氧化流反应器 (OFR) 中的活塞流程度：潜在气溶胶质量 (PAM) 反应器的研究

• DOI: 10.5194/amt-11-1741-2018
• 发表时间: 2017-11-29
• 期刊: Atmospheric Measurement Techniques
• 影响因子: 3.8
• 作者: Dhruv Mitroo;Yujian Sun;D. Combest;Purushottam Kumar;B. Williams
• 通讯作者: B. Williams