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

• 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

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，化学系的化学催化项目资助杜克大学的刘杰博士发展对等离子体激元的全面的基本理解。可再生能源，如用于化学制造的太阳能，将对化学工业的未来产生重大影响。当纳米粒子与光相互作用时，就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著影响表面化学反应的方式。等离子体催化是催化的一个新方向，它从太阳捕获光能，并利用它来加速重要的化学反应。然而，等离子体激元催化的机制是复杂的，因为光也加热纳米颗粒表面。分离热（简单加热）和表面等离子体对所观察到的化学反应的贡献是重要的基本理解。只有有了这样的理解，研究人员才能设计出最大效率地利用太阳光的系统。刘博士和他的团队正在开发实验方法来区分这些热效应和电子效应。拟议研究的结果为等离子体催化背后的机制提供了更深入的理解。此外，刘博士还专注于利用等离子体催化将二氧化碳转化为甲烷和甲醇等增值化学品。这种方法可以用来关闭碳循环，理想情况下，这种一碳燃料的使用和减少捕获导致净零碳排放。在这个项目中，刘博士正在促进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。刘博士积极参与北卡罗来纳州美国化学学会（ACS）项目SEED计划通过在暑假和学年期间接待来自代表性不足群体的高中生，鼓励他们成为未来的研究科学家。杜克大学的刘杰博士正在通过对CO2还原反应的综合宏观动力学研究，纳米结构铑表面反应动力学的光谱研究，通过理论分析进行指导和解释。一旦理解，在光催化反应中的等离子体速率增强和选择性控制的潜力可以被确定为各种各样的等离子体材料。此外，了解光热和非热效应（例如热电子介导的催化过程）的贡献不仅可以澄清机制，还可以使研究人员考虑设计更有效地利用太阳能的过程。刘博士参加了北卡罗来纳州美国化学学会（ACS）项目种子计划，在夏季和学年期间接待来自代表性不足群体的高中生。该项目的学生与研究生和刘博士一起设计和执行科学实验。该项目旨在支持高中生探索他们对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的法定使命，并通过使用基金会的智力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

High entropy spinel oxide for efficient electrochemical oxidation of ammonia

• DOI: 10.1007/s12274-021-3665-8
• 发表时间: 2021-07-01
• 期刊: NANO RESEARCH
• 影响因子: 9.9
• 作者: He, Shi;Somayaji, Vasishta;Liu, Jie
• 通讯作者: Liu, Jie