Molecular Photonic Materials

分子光子材料

基本信息

批准号：
1800022
负责人：
Gerald Meyer
金额：
$ 54.99万
依托单位：
University of North Carolina at Chapel Hill
依托单位国家：
美国
项目类别：
Continuing Grant
财政年份：
2018
资助国家：
美国
起止时间：
2018-08-01 至 2023-07-31
项目状态：
已结题

来源：
https://www.nsf.gov/awardsearch/showAward?AWD_ID=1800022&HistoricalAwards=false
关键词：
Molecular Photonic Materials

项目摘要

In this project, funded by the Chemical Structure, Dynamic & Mechanism B Program of the Chemistry Division, Professor Gerald Meyer of the Department of Chemistry at the University of North Carolina at Chapel Hill is characterizing intermolecular electron transfer reactions for molecules anchored to metal oxide surfaces. The goal of this research is to exploit self-exchange reactions as a means to transport charge across oxide surfaces for applications in optoelectronic devices, namely for the conversion of solar energy into stored chemical energy or electricity (e.g. dye-sensitized solar cells). The project lies at the interface of physical organic, inorganic, and materials chemistry, and is therefore well suited to the education of scientists at all levels. This group is also well-positioned to provide the highest level of education and training for students underrepresented in science. Outreach activities to grade school students in local and rural North Carolina are also part of the funded project. Research has shown that photo-oxidized dye molecules anchored to the sensitized mesoporous nanocrystalline (anatase) TiO2 thin films commonly used for dye-sensitized solar cells undergo self-exchange intermolecular electron transfer reactions (termed hole-hopping) with dynamics and efficiencies that can be tuned at the molecular level. These findings provide an opportunity to transport charges to desired locations without a loss in Gibbs free energy. Particular focus wiis being given to address the following fundamental questions: How can molecular structure be tuned to control intermolecular electron transfer? Is there a correlation between self-exchange reactions in fluid solution and those on oxide surfaces? Does self-exchange electron transfer between dyes influenced unwanted recombination reactions? Can self-exchange with molecules that contain two (or more) redox active groups be controlled by the bridge that links them? A kinetic approach that enables redox equilibria at the adiabatic/non-adiabatic border to be quantified for the first time is being utilized. The desired electron transfer chemistry is being initiated by pulsed light excitation or with an applied potential and quantified by in situ spectro-electrochemistry, absorption anisotropy, chronoabsorptometry, and transient absorption spectroscopy.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.

在该项目中，由化学部化学结构、动力学和机理 B 项目资助，北卡罗来纳大学教堂山分校化学系的 Gerald Meyer 教授正在表征锚定在金属氧化物表面的分子的分子间电子转移反应。这项研究的目标是利用自交换反应作为跨氧化物表面传输电荷的手段，用于光电器件中的应用，即将太阳能转化为储存的化学能或电能（例如染料敏化太阳能电池）。该项目位于物理有机、无机和材料化学的交汇处，因此非常适合各级科学家的教育。该群体也有能力为科学领域代表性不足的学生提供最高水平的教育和培训。针对北卡罗来纳州当地和农村地区小学生的外展活动也是该资助项目的一部分。研究表明，固定在常用于染料敏化太阳能电池的敏化介孔纳米晶（锐钛矿）TiO2 薄膜上的光氧化染料分子会发生自交换分子间电子转移反应（称为空穴跳跃），其动力学和效率可在分子水平上进行调整。这些发现提供了将电荷传输到所需位置而不损失吉布斯自由能的机会。特别关注解决以下基本问题：如何调整分子结构来控制分子间电子转移？流体溶液中的自交换反应与氧化物表面上的自交换反应之间是否存在相关性？染料之间的自交换电子转移是否会影响不需要的重组反应？与含有两个（或多个）氧化还原活性基团的分子的自交换可以通过连接它们的桥来控制吗？首次采用了一种动力学方法，能够量化绝热/非绝热边界的氧化还原平衡。所需的电子转移化学通过脉冲光激发或施加电势引发，并通过原位光谱电化学、吸收各向异性、计时吸收测量法和瞬态吸收光谱进行量化。该奖项反映了 NSF 的法定使命，并被认为值得通过以下方式获得支持：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。

项目成果

期刊论文数量（13）

专著数量（0）

科研奖励数量（0）

会议论文数量（0）

专利数量（0）

Influence of 4 and 4′ Substituents on Ru III/II Bipyridyl Self-Exchange Electron Transfer Across Nanocrystalline TiO 2 Surfaces

4 和 4-取代基对纳米晶 TiO 2 表面 Ru III/II 联吡啶自交换电子转移的影响

DOI：
10.1021/acs.jpcc.8b05281
发表时间：
2018
期刊：
The Journal of Physical Chemistry C
影响因子：
0
作者：
Motley, Tyler C.;Brady, Matthew D.;Meyer, Gerald J.
通讯作者：
Meyer, Gerald J.

Intramolecular Electronic Coupling Enhances Lateral Electron Transfer across Semiconductor Interfaces

分子内电子耦合增强了半导体界面上的横向电子转移

DOI：
10.1021/acs.jpcc.8b04836
发表时间：
2018
期刊：
The Journal of Physical Chemistry C
影响因子：
0
作者：
Motley, Tyler C.;Meyer, Gerald J.
通讯作者：
Meyer, Gerald J.

Ligand Control of Supramolecular Chloride Photorelease

超分子氯化物光释放的配体控制

DOI：
10.1021/acs.inorgchem.8b00559
发表时间：
2018
期刊：
Inorganic Chemistry
影响因子：
4.6
作者：
Turlington, Michael D.;Troian-Gautier, Ludovic;Sampaio, Renato N.;Beauvilliers, Evan E.;Meyer, Gerald J.
通讯作者：
Meyer, Gerald J.

Photocatalyst Assemblies with Two Halide Ions