CAS: Collaborative Research: Design, Characterization, and Modeling of Metal Nanocluster Electrocatalysts Linked to Three-Dimensional Graphene

CAS：合作研究：与三维石墨烯相关的金属纳米团簇电催化剂的设计、表征和建模

• 批准号: 2247574
• 负责人: Kwok-Fan Chow
• 金额: $ 47.22万
• 依托单位: University of Massachusetts Lowell
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2023
• 资助国家: 美国
• 起止时间: 2023-07-01 至 2026-06-30
• 项目状态: 未结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=2247574&HistoricalAwards=false
• 关键词: CAS; Collaborative; Research; Design; Characterization

With support of the Chemical Structure, Dynamics & Mechanisms-B Program of the Division of Chemistry, Kwok-Fan Chow, Jerome Delhommelle, and Mingdi Yan of the Department of Chemistry at the University of Massachusetts Lowell and Gonghu Li of the Department of Chemistry at the University of New Hampshire are developing new classes of graphene-supported nanocomposite materials for electrocatalytic applications. The goal of this research is to develop a new strategy for constructing electrocatalysts from metal nanoclusters (MNCs) and pristine graphene for electrochemical CO2 reduction. Knowledge gained through the proposed research is expected to improve our fundamental understanding of how the solid-solid interface impacts the electrocatalytic properties of nanocomposites. Such understanding could guide the design and fabrication of innovative devices for renewable energy applications. This project will provide excellent training opportunities for undergraduate and graduate researchers, promoting the participation of women and underrepresented minorities in STEM (science, technology, engineering and mathematics) research. This project also includes outreach activities (multiple one-day workshops at both institutions) designed for K-12 students to increase the national talent pipeline in nanoscience, chemistry, and materials science disciplines.Graphene-supported nanocomposite materials have attracted increasing interest among researchers due to their potential applications in various areas including catalysis. However, in graphene-based nanocomposite catalysts, the solid-solid interfaces between catalysts and graphene are often poorly defined. Understanding and optimizing such interfaces is particularly important for electrocatalytic applications such as CO2 reduction, in which electrons need to migrate from the graphene electrode to the catalyst. Molecular functionalization of graphene offers enormous opportunities to prepare new electrocatalysts (particularly MNCs) with enhanced electron transfer kinetics. Using gold nanoclusters (AuNCs) as the model MNCs, this project aims to develop a new strategy for constructing innovative electrocatalysts from MNCs and pristine graphene. Specifically, AuNCs will be covalently attached onto three-dimensional pristine graphene (3DG) electrodes through a series of rationally designed molecular linkers. This project requires complementary expertise from four research groups. A combination of synthesis, computational modeling, electrochemistry, and spectroscopy will be employed to investigate how the linker structure affects the performance of the AuNC-3DG electrocatalytic CO2 reduction. It is anticipated that the results obtained will enhance our fundamental understanding of how control over solid-solid interfaces at the molecular level impacts the performance of nanocomposite materials in electrochemical devices.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.

借助化学结构，动力学和机制-B化学划分，Kwok-Fan Chow，Jerome Delhommelle和Massachusetts Lowell大学化学系和新罕布什尔大学化学系化学系的Mingdi Yan正在开发新罕布什尔大学的应用程序材料的新型材料材料。这项研究的目的是制定一种新的策略，用于从金属纳米簇（MNC）和原始石墨烯中构建电催化剂，以减少电化学二氧化碳。预计通过拟议的研究获得的知识将提高我们对固体界面如何影响纳米复合材料的电催化特性的基本理解。这种理解可以指导可再生能源应用的创新设备的设计和制造。该项目将为本科和研究生研究人员提供极好的培训机会，促进妇女和代表性不足的STEM（科学，技术，工程和数学）研究的参与。该项目还包括为K-12学生而设计的外展活动（在这两个机构的多个为期一天的研讨会），旨在增加纳米科学，化学和材料科学学科的国家人才管道。Graphene支持的纳米复合材料因其在包括各种领域的潜在应用在内的研究人员而引起了越来越多的研究人员的兴趣。然而，在基于石墨烯的纳米复合催化剂中，催化剂和石墨烯之间的固体界面通常很差。理解和优化此类界面对于电催化应用（例如二氧化碳还原）尤为重要，其中电子需要从石墨烯电极迁移到催化剂。石墨烯的分子功能化提供了巨大的机会，可以用增强的电子传递动力学制备新的电催化剂（尤其是MNC）。该项目使用金纳米簇（AUNC）作为型号MNC，旨在制定一种新的策略，用于构建MNCS和原始石墨烯的创新电催化剂。具体而言，通过一系列理性设计的分子接头将AUNC共价连接到三维原始石墨烯（3DG）电极上。该项目需要四个研究小组的补充专业知识。合成，计算建模，电化学和光谱法的结合将用于研究接头结构如何影响AUNC-3DG电催化CO2还原的性能。可以预料，获得的结果将增强我们对分子水平上固体界面的控制如何影响纳米复合材料在电化学设备中的性能。该奖项反映了NSF的法定任务，并通过评估该基金会的智力优点和广泛的影响来评估NSF的法定任务，并被视为值得进行的支持。