SusCHEM: Collaborative Research: Decoupling Structure and Surface Chemistry Impacts of Carbon Nanomaterials on Environmentally Relevant Electrochemical and Biological Activity

PI：Gilbertson，Leanne/Francois Perreault计划号：1709031/1708681纳米材料是在分子水平上进行设计的，以改变其结构和功能特性，这反过来又使创新的纳米使能技术的发展成为可能。然而，这些同样的性质操纵有可能影响这些工程纳米材料的不利影响。因此，推动安全和功能纳米产品的开发至关重要。这是通过确定材料结构特征、物理化学性质、功能和危害之间的关系来实现的。这些已建立的关系可以用来指导合理的可持续材料设计。这一方法将在这个项目中应用于碳纳米材料，这是工程纳米材料的领先类别之一(基于生产量)。它们的高比表面积、电子性质和控制表面化学的能力使许多环境应用成为可能，例如，利用碳纳米材料与环境介质的相互作用来检测、去除或降解污染物。要实现这些下一代应用的性能，同时排除对环境的负面影响，就必须从根本上了解引起理想和不良反应的材料特性。这些研究工作将：(I)确定合成高性能碳纳米材料的设计参数，考虑结构和表面化学；(Ii)确定与碳纳米材料表面化学、固有结构、电化学和生物活性有关的机理；以及(Iii)建立参数关系，确定如何在对固有材料危险影响最小的情况下选择性地改善电化学活性。拟议工作的更广泛影响将影响三个关键领域：(I)发展对理解纳米材料在其应用中和环境中相互作用的现象至关重要的基本科学概念；(Ii)加快我们和其他人在整个科学和工程界的本科生和研究生教育方面的努力；(Iii)通过培训准备好的内容模块，促进K-12科学教育工作者的专业发展，将通过调查监测其成功情况，以评估学生的参与度和学习成果。拟议项目的科学目标是解决材料表面的分子水平现象，这些现象支配着包括碳纳米管和石墨烯在内的不同同素异形体的碳纳米材料的化学和生物活性。中心假设是表面官能团和主体碳材料之间的相互作用是重要的，并将对不同的碳纳米结构产生独特的影响。了解表面化学对具有内在不同电子结构的碳纳米材料的反应性的作用“半导体和金属碳纳米管和石墨烯”可以阐明设计参数以适应材料的功能。该项目的基本原理是，通过建立包括宿主碳纳米材料的化学性质的参数关系，可以极大地提高碳纳米启用的电子和电化学应用的性能。此外，为了安全地实现碳纳米材料的应用，有必要从机理上了解分子水平的操纵如何影响其内在性质。预期的研究成果是：(1)以参数关系(结构-性质-功能和结构-性质-危险)的形式建立材料设计参数，这将为功能和安全的碳纳米产品的开发提供信息；(2)通过解决基本的化学性质以及与与环境有关的生物系统的相互作用，提高对碳纳米材料电化学和生物反应性的基本作用机制的理解；(3)确定已建立的参数关系受环境条件调节的程度，为确定在实验室条件下建立的关系的稳健性提供途径。

PI: Gilbertson, Leanne / Francois Perreault Proposal Number: 1709031 / 1708681 Nanomaterials are engineered at the molecular level to modify their structure and functional properties, which in turn, enables the development of innovative nano-enabled technologies. However, these same property manipulations have the potential to influence the adverse impacts of these engineered nanomaterials. It is therefore, critically important to drive the development of safe and functional nano-enabled products. This is accomplished through the identification of relationships between material structural features, physicochemical properties, functions, and hazards. These established relationships can then be used to inform rational sustainable material design. This approach will be applied in this project to carbon nanomaterials, which are one of the leading classes of engineered nanomaterials (based on production volumes). Their high surface area, electronic properties, and the ability to control the surface chemistry enable numerous environmental applications where the interactions of the carbon nanomaterial with environmental media are used to detect, remove, or degrade contaminants, for example. Realizing the performance of these next generation applications while precluding negative environmental impacts necessitates a fundamental understanding of the material properties that elicit both desirable and undesirable responses. These research efforts will: (i) identify design parameters for the synthesis of high performance carbon nanomaterials, taking into account structure and surface chemistry, (ii) define mechanisms that relate carbon nanomaterial surface chemistry, inherent structure, electrochemical and biological activity, and (iii) establish parametric relationships that identify how electrochemical activity can be selectively improved with minimal impact on inherent material hazard. The broader impacts of the proposed work will influence three key areas: (i) the development of fundamental scientific concepts crucial to understanding phenomena driving the interactions of nanomaterials in their applications and in the environment, (ii) accelerate the efforts of us and others in the education of undergraduate and graduate students throughout the scientific and engineering communities, and (iii) the professional development of K-12 science educators through training of prepared content modules, the success of which will be monitored through surveys to evaluate student engagement and learning gains. The scientific objective of the proposed project is to resolve the molecular-level phenomena at the material surface that govern the chemical and biological reactivity of different allotropes of carbon nanomaterials, including carbon nanotubes and graphene. The central hypothesis is that the interplay between the surface functional group and the host carbon material is important and will present unique influences for different carbon nanostructures. Understanding the role of surface chemistry on the reactivity of carbon nanomaterials with inherently different electronic structure "semiconducting and metallic carbon nanotubes and grapheme" can elucidate design parameters to tailor the material functionality. The project rationale is that the performance of carbon nano-enabled electronic and electrochemical applications can be greatly improved through the establishment of parametric relationships that include the chemical nature of the host carbon nanomaterial. Furthermore, to safely enable carbon nanomaterial applications, it is necessary to gain a mechanistic understanding of how molecular level manipulations influence their intrinsic properties. The expected research outcomes are to (i) establish material design parameters, in the form of parametric relationships (structure-property-function and structure-property-hazard), that will inform the development of functional and safe carbon nano-enabled products, (ii) provide enhanced understanding of the underlying mechanisms of action of carbon nanomaterial electrochemical and biological reactivity by resolving the fundamental chemical properties and interactions with environmentally-relevant biological systems, and (iii) determine the extent to which the established parametric relationships are modulated by environmental conditions, providing an avenue towards determining the robustness of the relationships established under laboratory conditions.