Heterogeneous Catalysis on Plasmonic Metallic Nanostructures: Selective Catalytic Conversion at Lower Temperatures co-Driven by Solar and Thermal Energy

等离激元金属纳米结构的多相催化：太阳能和热能共同驱动的较低温度下的选择性催化转化

• 批准号: 1362120
• 负责人: Suljo Linic
• 金额: $ 42万
• 依托单位: Regents of the University of Michigan - Ann Arbor
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2014
• 资助国家: 美国
• 起止时间: 2014-10-01 至 2018-09-30
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1362120&HistoricalAwards=false
• 关键词: Heterogeneous; Catalysis; Plasmonic; Metallic; Nanostructures

In this project funded by the Chemical Catalysis program of the Chemistry Division, Professor Suljo Linic of The University of Michigan (Ann Arbor) is developing a new generation of photocatalysts that use solar energy to drive chemical transformation. These new photocatalysts are small nanoparticles of silver, copper and gold, which are on one hand characterized by their strong interaction with solar light (i.e., these concentrate the solar energy) and on the other hand by their high chemical activity (i.e., activate a number of desired chemical transformations). This new generation of photocatalysts will complement semiconductor photocatalysts, which are traditionally used in this field. An outreach program developed by Professor Linic to area high schools is allowing local high school students the opportunity to participate in this research and to learn about sustainable energy transformations. The broader impacts of this work include potential societal benefits from the discovery of new generation of photocatalysts as well as the development of training opportunities for students and teachers. It was demonstrated recently that when illuminated with low intensity light, plasmonic metal nanoparticles can activate electron-driven chemical reactions at meaningful rates. The characteristic of plasmonic nanostructures (Ag, Au, and Cu were used) that makes them fundamentally different than extended metal surfaces (metal bulk), is their strong resonant interaction with UV-vis light through the excitation of localized surface plasmon resonance (LSPR). While these initial studies led to a very vibrant field of photochemistry on plasmonic metals, there are many unanswered critical issues. The project focuses on a number of these issues, including identification of: (i) the mechanism by which plasmons transfer energetic electrons to the adsorbates and in doing so induce chemical transformations, (ii) the mechanisms responsible for the reported non-linear dependency between reaction rate and light intensity, and (iii) the nature of the active sites responsible for the observed photochemistry on plasmonic metal nanoparticles. Addressing these issues is critical for the development of predictive relationships between optical properties of metal nanoparticles, their geometric structure (at the single particle and a cluster level), and their photocatalytic activity. This is important for our understanding of the surface photo-chemistry taking place on these materials, the extent to which these processes can be controlled, and the parameters that influence the design of optimal photo-catalytic systems.

在化学部化学催化计划资助的该项目中，密歇根大学（Ann Arbor）的Suljo Linic教授正在开发新一代的光催化剂，这些光催化剂使用太阳能驱动化学转化。这些新的光催化剂是银，铜和金的小纳米颗粒，其特征是它们与太阳能（即，这些都集中了太阳能），另一方面是通过其高化学活性（即激活许多所需的化学转化）的特征。这种新一代的光催化剂将补充半导体光催化剂，这些光催化剂传统上是在该领域中使用的。 Linic教授到地区高中开发的宣传计划允许当地高中学生有机会参加这项研究并了解可持续的能源转型。这项工作的更广泛影响包括发现新一代光催化剂以及为学生和教师创造培训机会的潜在社会利益。 最近证明，当用低强度的光照明时，等离子体金属纳米颗粒可以以有意义的速率激活电子驱动的化学反应。血浆纳米结构（使用Ag，Au和Cu）的特征使它们与扩展金属表面（金属散装）根本不同，是通过激发局部表面等离子体共振（LSPR）的激发，它们与UV-VIS光的强烈谐振相互作用（LSPR）。尽管这些最初的研究导致了等离子金属的光化学领域，但仍有许多未解决的关键问题。该项目侧重于许多此类问题，包括：（i）等离子体将能量电子传递到吸附物的机制，并在这样做的过程中诱导化学转化，（ii）负责在反应速率和光强度和光强度之间报告的非线性依赖性的机制，以及（iii）负责观察照片的活跃场所的性质，该机构是plassicic nis nan nan nan nan nan nan nan nan nan nan。解决这些问题对于金属纳米颗粒的光学性质，其几何结构（在单个粒子和簇水平上）及其光催化活性之间的预测关系至关重要。这对于我们了解这些材料上的表面光化学，可以控制这些过程的程度以及影响最佳光催化系统设计的参数很重要。