CAREER: Elucidation of the mechanistic origins of plasmon-induced chemical reactions

职业：阐明等离激元诱导的化学反应的机械起源

• 批准号: 1455011
• 负责人: Prashant Jain
• 金额: $ 65.56万
• 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: 2015
• 资助国家: 美国
• 起止时间: 2015-08-01 至 2023-02-28
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1455011&HistoricalAwards=false
• 关键词: CAREER; Elucidation; mechanistic; origins; plasmon

With this CAREER Award, the Macromolecular, Supramolecular and Nanochemistry Program of the Division of Chemistry is supporting Professor Prashant Jain of the University of Illinois to study the detailed manner in which light energy is converted into chemical energy within metallic materials. This process, if properly understood and controlled, may become a candidate technology for capturing solar energy and for driving energy-intensive processes in the chemical industry with light. Professor Jain aims at preparing strongly light-absorbing materials that can efficiently convert sunlight into chemical energy in fuels. Another effort involves the achievement of light-to-chemical energy conversion using cheaper, more abundant materials. Alongside the laboratory efforts, an interactive software tool is being developed and employed for the purpose of education on the interaction of light with matter. The educational program is aimed at generating early scientific interest in the classroom by means of vivid, hands-on examples from optics, preparing high school, undergraduate, and graduate students for future science and technology careers. Outreach activities seek to foster community awareness of solar energy as a clean, renewable alternative to energy from fossil fuels. Professor Jain investigates the physicochemical mechanism(s) by which the plasmonic excitation of a noble metal-containing heterostructure induces or catalyzes chemical reactions on the surface of the nanostructure. In this project, a plasmonic heterostructure consisting of Au nanoparticles in contact with a semiconducting oxide (titanium dioxide and zinc oxide) is studied for determining the relative contributions of plasmonic near-field enhancement, hot electron transfer, and photothermal heating in photocatalytic reactions. This research aims to elucidate the mechanistic role of the oxide and assess whether near-field-assisted bandgap or sub-bandgap photoexcitation of carriers in the oxide is responsible for the observed photoactivity, or, whether charge separation across the metal/oxide is a more important contributor. Professor Jain uses single-molecule fluoresence to identify whether the photoreaction takes place on the metal, on the semiconducting oxide, or at the metal/oxide interface. Finally, he explores plasmon excitation-induced photocatalysis in a noble metal-free plasmonic oxide, which represents an interface-free system where plasmonic excitation and semiconductor electronic transitions are localized within the same crystallite.

凭借这一职业奖，化学系的高分子、超分子和纳米化学项目正在支持伊利诺伊大学的 Prashant Jain 教授研究光能在金属材料内转化为化学能的详细方式。如果正确理解和控制这一过程，可能会成为捕获太阳能和用光驱动化学工业中能源密集型过程的候选技术。 Jain教授的目标是制备强吸光材料，能够有效地将阳光转化为燃料中的化学能。 另一项努力涉及使用更便宜、更丰富的材料实现光能到化学能的转换。除了实验室的努力之外，还开发并使用了一种交互式软件工具，用于光与物质相互作用的教育目的。该教育计划旨在通过生动的光学实践示例在课堂上激发早期的科学兴趣，为高中生、本科生和研究生未来的科学和技术职业做好准备。外展活动旨在提高社区对太阳能作为化石燃料能源的清洁、可再生替代能源的认识。 Jain 教授研究了含贵金属异质结构的等离子体激发诱导或催化纳米结构表面化学反应的物理化学机制。在该项目中，研究了由与半导体氧化物（二氧化钛和氧化锌）接触的金纳米粒子组成的等离子体异质结构，以确定光催化反应中等离子体近场增强、热电子转移和光热加热的相对贡献。这项研究旨在阐明氧化物的机械作用，并评估氧化物中载流子的近场辅助带隙或亚带隙光激发是否是造成观察到的光活性的原因，或者金属/氧化物上的电荷分离是否更重要。重要贡献者。 Jain 教授使用单分子荧光来识别光反应是否发生在金属、半导体氧化物或金属/氧化物界面上。最后，他探索了不含贵金属的等离激元氧化物中的等离激元激发诱导的光催化作用，该氧化物代表了一种无界面系统，其中等离激元激发和半导体电子跃迁位于同一微晶内。

项目成果

Activation Energies of Plasmonic Catalysts

等离激元催化剂的活化能

• DOI: 10.1021/acs.nanolett.6b01373
• 发表时间: 2016-05
• 期刊: Nano Letters
• 影响因子: 10.8
• 作者: Kim, Youngsoo;Dumett Torres, Daniel;Jain, Prashant K.
• 通讯作者: Jain, Prashant K.