Collaborative Research: CAS-Climate: Structure, Dynamics, and Reaction Mechanism of Supported Single Atom for Photocatalytic CO2 Reduction

合作研究：CAS-气候：光催化CO2还原的负载单原子的结构、动力学和反应机制

• 批准号: 2154837
• 负责人: Jing Gu
• 金额: $ 26.88万
• 依托单位: San Diego State University Foundation
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2022
• 资助国家: 美国
• 起止时间: 2022-08-01 至 2025-07-31
• 项目状态: 未结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=2154837&HistoricalAwards=false
• 关键词: Collaborative; Research; CAS; Climate; Structure

With support from the Chemical Structure, Dynamics & Mechanisms-B (CSDM-B) Program of the Chemistry Division, Jier Huang of the Department of Chemistry at Marquette University and Jing Gu of the Department of Chemistry and Biochemistry at San Diego State University aim to construct and investigate new generation single atom catalysts for visible light driven carbon dioxide (CO2) reduction to form chemical fuels with high efficiency, selectivity, and stability. Photocatalytic CO2 reduction through the harnessing solar energy represents one of the most attractive strategies that attempts to simultaneously address the greenhouse gas sequestration issue and work toward alternative energy sources for the future. The research will be supplemented by diverse educational and outreach activities, including efforts to encourage graduate and undergraduate students, especially members of underrserved minority groups, to consider pursuing careers in science. The Huang/Gu team will also provide opportunities for students/teachers ranging from elementary to high schools to advance their general understanding of catalysis and renewable energy technologies. Supported single atoms (SAs) have emerged as a novel class of catalysts, offering new promise for light-driven CO2 reduction. The focus of prior research is largely on documenting the efficiency, stability, and the selectivity of the catalysts, not the fundamental mechanistic studies that underlines the correlation of SA structure and their photocatalytic performance. To address such gaps in knowledge, Drs. Gu and Professor Huang are targeting the following objectives by leveraging their complementary expertise in materials design and synthesis with time resolved spectroscopy: 1) to systematically tune the geometric and electronic structures of supported SAs by altering the intrinsic nature of SAs, the metal-support interaction, and by comparing with nanoparticles with various sizes; 2) to examine the charge separation and structural dynamics, and resolving the intermediate structures at catalytic active sites with high temporal and spatial resolution using time resolved optical and X-ray absorption spectroscopy; and 3) to evaluate the direct correlation of the structures of the supported SA catalysts with their photophysical properties and catalytic function to establish structure-property-function relationships for CO2 reduction. Results obtained from these efforts are expected to aid in the development of more effective supported SAs for photocatalytic CO2 reduction, going forward.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.

在化学系化学结构、动力学与机理-B（CSDM-B）项目的支持下，马凯特大学化学系的黄继尔和圣地亚哥州立大学化学与生物化学系的谷晶旨在构建和研究新一代单原子催化剂，用于可见光驱动的二氧化碳（CO2）还原，以形成高效、选择性和稳定性的化学燃料。通过利用太阳能进行光催化二氧化碳减排是最具吸引力的策略之一，它试图同时解决温室气体封存问题并致力于未来的替代能源。 该研究将得到多样化的教育和外展活动的补充，包括鼓励研究生和本科生，特别是服务不足的少数群体成员考虑从事科学事业。 黄/顾团队还将为从小学到高中的学生/教师提供机会，以加深他们对催化和可再生能源技术的一般理解。负载型单原子 (SA) 已成为一类新型催化剂，为光驱动二氧化碳减排提供了新希望。先前研究的重点主要是记录催化剂的效率、稳定性和选择性，而不是强调SA结构与其光催化性能之间的相关性的基本机理研究。为了解决这种知识差距，博士。顾和黄教授利用他们在材料设计和时间分辨光谱合成方面的互补专业知识，致力于实现以下目标：1）通过改变SA的本质、金属-载体相互作用以及与不同尺寸的纳米颗粒进行比较，系统地调整负载SA的几何和电子结构； 2）检查电荷分离和结构动力学，并使用时间分辨光学和X射线吸收光谱以高时间和空间分辨率解析催化活性位点的中间结构； 3）评估负载型SA催化剂的结构与其光物理性质和催化功能的直接相关性，以建立CO2还原的结构-性能-功能关系。 从这些努力中获得的结果预计将有助于开发更有效的支持型 SA，用于光催化二氧化碳减排。该奖项反映了 NSF 的法定使命，并通过使用基金会的智力优点和更广泛的影响审查标准进行评估，被认为值得支持。