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.

在这个由化学结构，动力学和机制B计划资助的合作项目中，Marquette大学化学系的Jier Huang教授和圣地亚哥州立大学化学系教授的旨在构建和调查新一代的单个Atom Atom Catalyst，以实现可见的轻型光驱动型二氧化碳（CO2）的效率（CO2）的效率，以适应高度效率，以供应化学效率，并效率高。通过利用太阳能来减少光催化二氧化碳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。 这项研究得到了多种教育和外展活动的补充，包括鼓励研究生和本科生，尤其是代表性不足的少数群体，从事STEM研究的职业，并为从基础到高中的学生/老师提供机会，以促进他们对催化和可再生能源技术的一般理解。受支持的单个原子（SAS）已成为一种新型的催化剂，为轻度驱动二氧化碳提供了新的希望。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结构及其光催化性能的基本机械研究。为了解决知识的差距，GU教授和黄教授通过利用其在材料设计和合成方面的互补专业知识与时间分辨的光谱镜检查来针对以下目标：1）系统地调整支持SAS的几何和电子结构，通过改变SAS的内在性质，与金属辅助互动的互动，以及与Metal-Pplorts Interaction与Nananaipsison进行比较，以改变SAS的几何和电子结构。 2）使用时间分辨的光学和X射线吸收光谱检查，检查电荷分离和结构动力学，并在具有高时间和空间分辨率的催化活性位点上解决中间结构； 3）评估受支持的SA催化剂的结构与其光物理特性和催化功能的直接相关性，以建立结构 - 螺纹功能关系以减少CO2。 从这些努力中获得的结果将在为减少光催化二氧化碳减少的更有效支持的SAS开发更有效的SAS方面具有重要价值。该奖项反映了NSF的法定任务，并使用基金会的知识分子优点和更广泛的影响评估标准，认为值得通过评估来获得支持。

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