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: 2321203
• 负责人: Jier Huang
• 金额: $ 26.93万
• 依托单位: Boston College
• 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: 2023-04-01 至 2025-07-31
• 项目状态: 未结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=2321203&HistoricalAwards=false
• 关键词: Collaborative; Research; CAS; Climate; Structure

In this collaborative project, funded by the Chemical Structure, Dynamics & Mechanisms B Program of the Chemistry Division, Professor Jier Huang of the Department of Chemistry at Marquette University and Professor Jing Gu of the Department of Chemistry 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 by harnessing solar energy represents one of the most attractive strategies that may simultaneously address the global warming issue and fulfill the future energy demand. The research is supplemented by diverse educational and outreach activities, including encouraging graduate and undergraduate students, especially underrepresented minority groups, into careers in STEM research, and providing 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, Professor Gu and Professor Huang target the following objectives by leveraging their complementary expertise in materials design and synthesis with time resolved spectroscopy: 1) systematically tuning the geometric and electronic structures of supported SAs via altering the intrinsic nature of SAs, the metal-support interaction, and the comparison with nanoparticles with various sizes; 2) examining 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) evaluating 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 will be of significant value in developing more effective supported SAs for photocatalytic CO2 reduction.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.

在这个由化学系化学结构，动力学机制B计划资助的合作项目中，马奎特大学化学系的Jier Huang教授和圣地亚哥州立大学化学系的Jing Gu教授旨在构建和研究新一代可见光驱动的二氧化碳（CO2）还原的单原子催化剂，以形成高效，选择性和稳定的化学燃料。通过利用太阳能的光催化CO2还原是最有吸引力的策略之一，可以同时解决全球变暖问题并满足未来的能源需求。 该研究还辅以各种教育和推广活动，包括鼓励研究生和本科生，特别是代表性不足的少数群体，进入STEM研究的职业生涯，并为从小学到高中的学生/教师提供机会，以提高他们对催化和可再生能源技术的一般理解。支持的单原子（SA）已成为一类新型催化剂，为光驱动的二氧化碳减排提供了新的希望。现有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相关性的基本机理研究。为了弥补这些知识上的差距，顾教授和黄教授利用他们在材料设计和合成方面的互补专业知识，利用时间分辨光谱实现了以下目标：1）通过改变SA的固有性质，金属-载体相互作用以及与不同尺寸的纳米颗粒的比较，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分辨催化活性位点处的中间体结构;和3）评价负载型SA催化剂的结构与其物理化学性质和催化功能的直接相关性，以建立CO2减排的结构-性质-功能关系。 从这些努力中获得的结果将在开发更有效的支持SA的光催化CO2 reduction方面具有重要价值。该奖项反映了NSF的法定使命，并通过使用基金会的知识价值和更广泛的影响审查标准进行评估，被认为值得支持。

项目成果

Nanomaterials and Sustainability

纳米材料与可持续性

• DOI: 10.1021/acsenergylett.3c01303
• 发表时间: 2023
• 期刊: ACS Energy Letters
• 影响因子: 22
• 作者: Wiederrecht, Gary P.;Bachelot, Renaud;Xiong, Hui;Termentzidis, Konstantinos;Nominé, Alexandre;Huang, Jier;Kamat, Prashant V.;Rozhkova, Elena A.;Sumant, Anirudha;Ostraat, Michele
• 通讯作者: Ostraat, Michele