Maximizing the Harvesting of Photogenerated Electron-Hole Pairs in Hybrid Plasmonic Nanosystems

最大化混合等离子体纳米系统中光生电子空穴对的收获

• 批准号: 2304910
• 负责人: Prashant Jain
• 金额: $ 44.17万
• 依托单位: University of Illinois at Urbana-Champaign
• 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: 2023-06-15 至 2026-05-31
• 项目状态: 未结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=2304910&HistoricalAwards=false
• 关键词: Maximizing; Harvesting; Photogenerated; Electron; Hole

With support from the Macromolecular, Supramolecular and Nanochemistry Program (MSN) in the Division of Chemistry, Professor Prashant Jain of the University of Illinois Urbana-Champaign is developing materials, principles, and strategies for capturing visible light from solar radiation and deploying it in a directed and energy-efficient manner to form high-value chemical bonds. A particular target is the chemical bond between nitrogen and carbon atoms found in many high-value chemicals. Such light harvesting is currently achievable by nanometer-scale particles of coinage metals; however, the conversion of light to chemical energy is inefficient and uncontrolled. Professor Jain is addressing this challenge by using oxide minerals engineered on the nanometer scale to absorb visible light and produce energetic charges that survive long enough to be used productively for chemical energy generation. Furthermore, he is pairing these light-absorbing materials with chemical agents that direct and promote the flow of charge. If successful, the research will lead to technologies for manufacturing energetic reagents, fuels, and fine chemicals using renewable power and producing no carbon emissions. In public outreach activities, Professor Jain is also promoting sustainable technologies and practices through solar energy- and electricity-powered removal of nitrate pollutants from water sources near agriculture-dominated communities. The graduate students engaged in this project are gaining valuable experience in a wide range of chemical syntheses, spectroscopic and chemical kinetic analyses, and catalysis. This project is also providing opportunities for undergraduate researchers interested in sustainable technologies.Plasmonic nanostructures allow the harvesting of light in the form of energetic charge carriers, which can in turn be deployed to accelerate or drive chemical reactions. However, harvesting of light and light-to-chemical energy conversion via this scheme remains well below the thermodynamic efficiency limit. Professor Jain is applying a newer class of plasmonic materials and hybridization strategies for maximizing the separation of photogenerated electron–hole pairs and utilizing them more efficiently and selectively for reactions such as nitrogen–carbon bond formation. Specifically, Professor Jain is employing plasmonic metal oxide nanostructures, which are anticipated to exhibit slower carrier relaxation and recombination. The other strategies involve the hybridization of plasmonic metal oxide nanostructures with polar surfaces, water-oxidation promoters, and homogeneous catalysts. The work is expected to elucidate physicochemical and materials design factors that govern carrier separation and extraction and illustrate chemical architectures and schemes that are ideally suited for the directed and efficient flow of carriers on the nanoscale. These concepts coupled with the use of non-metallic plasmonic oxide nanostructures have the potential to expand the scope and reach of plasmonic chemistry for achieving energy-relevant chemical transformations.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.

在化学系高分子、超分子和纳米化学项目 (MSN) 的支持下，伊利诺伊大学厄巴纳-香槟分校的 Prashant Jain 教授正在开发从太阳辐射中捕获可见光并将其部署到应用中的材料、原理和策略。一种特定的目标是在许多高价值化学品中发现的氮和碳原子之间的化学键。造币金属的纳米级颗粒；然而，光到化学能的转换效率低且不受控制，贾恩教授正在通过使用纳米级设计的氧化物矿物来吸收可见光并产生存活足够长的高能电荷来解决这一挑战。此外，他正在将这些光吸收材料与引导和促进电荷流动的化学试剂配对，如果成功，该研究将带来用于制造高能试剂、燃料和精细化学品的技术。可再生在公共推广活动中，Jain 教授还推广通过太阳能和电力去除农业主导社区附近水源中的硝酸盐污染物的可持续技术和实践。该项目还为对可持续技术感兴趣的本科生研究人员提供了在各种化学合成、光谱和化学动力学分析以及催化方面的宝贵经验。等离激元纳米结构可以以高能电荷的形式收集光。然而，通过这种方案收集光和光到化学能的转换仍然远低于热力学效率极限。杂化策略可最大限度地分离光生电子-空穴对，并更有效地、选择性地利用它们进行氮-碳键形成等反应。其他策略涉及等离子体金属氧化物纳米结构与极性表面、水氧化促进剂和均相催化剂的杂化，这项工作预计将阐明控制载体分离和提取的物理化学和材料设计因素，并说明化学结构和方案。这些概念与非金属等离子体氧化物纳米结构的使用相结合，具有扩大范围和有效覆盖范围的潜力。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

The physics of plasmon-driven energy conversion

等离子体驱动的能量转换的物理学

• DOI: 10.1063/5.0168581
• 发表时间: 2023-08
• 期刊: The Journal of Chemical Physics
• 作者: Jain, Prashant K.;Kim, Zee Hwan;Wei, Wei David
• 通讯作者: Wei, Wei David

Watching Plasmon-Induced Nanoparticle Ostwald Ripening

观察等离激元诱导的纳米粒子奥斯特瓦尔德成熟

• DOI: 10.1021/acs.jpcc.3c04035
• 发表时间: 2023-08-09
• 期刊: The Journal of Physical Chemistry C
• 作者: Francis M. Alcorn;Maya Chattoraj;R. M. van der Veen;P. Jain
• 通讯作者: P. Jain