CAS: Understanding the Contributions from Both Thermal and Non-Thermal Factors in Plasmonic Catalysis

CAS：了解热因素和非热因素在等离激元催化中的贡献

基本信息

批准号：
1954838
负责人：
Jie Liu
金额：
$ 53万
依托单位：
Duke University
依托单位国家：
美国
项目类别：
Continuing Grant
财政年份：
2020
资助国家：
美国
起止时间：
2020-08-15 至 2024-04-30
项目状态：
已结题

来源：
https://www.nsf.gov/awardsearch/showAward?AWD_ID=1954838&HistoricalAwards=false
关键词：
CAS Understanding Contributions Both Thermal

项目摘要

With this award, the Chemical Catalysis Program of the Division of Chemistry is funding Dr. Jie Liu of Duke University to develop a comprehensive fundamental understanding of plasmonic photocatalysis. Renewable energy such as sunlight for chemical manufacturing will impact the future of the chemical industry significantly. When nanoparticles interact with light an electronic phenomenon known as a surface plasmon is created. These surface plasmons can significantly affect the way the surfaces chemically react. Plasmonic catalysis, a recent direction in catalysis, captures light energy from the sun and uses it to accelerate important chemical reactions. However, the mechanism of plasmonic catalysis is complicated because light also heats the nanoparticle surface. Separating the thermal (simple heating) and surface plasmon contributions to the observed chemical reactions is important to fundamental understanding. Only with such understanding will researchers be able to design systems to use sunlight at maximum efficiency. Dr. Liu and his team are developing experimental methods to distinguish these thermal and electronic effects. The results from the proposed research is providing deeper understanding of the mechanism behind plasmonic catalysis. In addition, Dr. Liu is focusing on converting CO2 to value-added chemicals such as methane and methanol using plasmonic catalysis. This approach could serve to close the carbon cycle, ideally resulting net zero carbon emission from the use and reductive capture of such one carbon fuels. In this project, Dr. Liu is fostering the engagement of female researchers as well as researchers from underrepresented minority groups. Dr. Liu is actively participating in the North Carolina American Chemical Society (ACS) Project SEED Program by hosting high school students from underrepresented groups during summers and the school yearencouraging them to become future research scientists.Dr. Jie Liu of Duke University is developing a comprehensive fundamental understanding of plasmonic photocatalysis through an integrated macroscopic kinetic study of the CO2 reduction reaction with targeted spectroscopic investigations of the reaction dynamics on the surface of nanostructured rhodium, guided and interpreted by theoretical analyses. Once understood, the potential for plasmonic rate enhancement and selectivity control in photocatalytic reactions may be ascertained for a large variety of plasmonic materials. In addition, understanding the contributions from photo-thermal as well as non-thermal effect (e.g. hot electrons mediated catalytic process) is not only clarifying the mechanism but also enabling researchers to consider designing processes for more efficient use of energy from sunlight. Dr. Liu participates in the North Carolina American Chemical Society (ACS) Project SEED Program by hosting high school students from underrepresented groups during summers and the school year. Students in the program work with graduate students and Dr. Liu to design and perform scientific experiments. This program is supporting high school students to explore their interest in STEM fields thereby encouraging them to become future researchers in these fields.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.

有了这个奖项，化学系的化学催化计划正在为杜克大学的李·刘博士提供资金，以对等离子光催化有全面的基本了解。可再生能源（例如用于化学制造的阳光）将对化学工业的未来产生重大影响。当纳米颗粒与光相互作用时，会产生一种称为表面等离子体的电子现象。这些表面等离子体可以显着影响表面化学反应的方式。等离子体催化是催化的最新方向，它捕获了来自太阳的光能，并使用它加速了重要的化学反应。然而，血浆催化的机理很复杂，因为光还加热了纳米颗粒表面。分离热（简单加热）和表面等离子体对观察到的化学反应的贡献对于基本理解很重要。只有有这样的理解，研究人员才能设计系统以最大程度地使用阳光。 Liu博士和他的团队正在开发实验方法，以区分这些热和电子效应。拟议的研究的结果是对等离子体催化背后的机制有了更深入的了解。此外，Liu博士使用等离子体催化剂将CO2转化为甲烷和甲醇等增值化学物质。这种方法可以用来关闭碳循环，理想情况下，由于使用和还原捕获了这种一种碳燃料，因此净零碳排放。在这个项目中，刘博士正在培养女性研究人员以及代表性不足的少数群体的研究人员的参与。 Liu博士通过在夏季和学年期间接待来自代表性不足的小组的高中生，使他们成为未来的研究科学家。杜克大学的Jie Liu通过对纳米结构的Rhodium表面上的反应动力学的靶向光谱研究对CO2还原反应进行的宏观动力学研究进行了综合的宏观动力学研究，从而对等离子体光催化的基本了解进行了全面的基本了解，并通过理论分析来解释并解释了纳米结构的Rhodium表面。一旦理解，可以确定各种等离激元材料的光催化反应中等离子体速率增强和选择性控制的潜力。此外，了解光热以及非热效应（例如热电子介导的催化过程）的贡献不仅阐明了该机制，而且还使研究人员能够考虑设计过程，以从阳光中更有效地利用能量。刘博士通过在夏季和学年接待来自代表性不足的小组的高中生，参加了北卡罗来纳州美国化学学会（ACS）项目种子计划。该课程的学生与研究生和Liu博士一起设计和执行科学实验。该计划支持高中学生探索他们对STEM领域的兴趣，从而鼓励他们成为这些领域的未来研究人员。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审查标准，认为值得通过评估来获得支持。