Excellence in Research: Investigation of Small Molecule Adsorption and Conversion on the Semiconductor/Ionic-Liquid Interface and Application to Sensing and Catalysis

卓越研究：半导体/离子液体界面上小分子吸附和转化的研究及其在传感和催化方面的应用

• 批准号: 1832167
• 负责人: Kevin Riley
• 金额: $ 69.98万
• 依托单位: Xavier University of Louisiana
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2018
• 资助国家: 美国
• 起止时间: 2018-09-01 至 2023-08-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1832167&HistoricalAwards=false
• 关键词: Excellence; Research; Investigation; Small; Molecule

The detection of small gas molecules is extremely important in industrial, environmental, and other applications. Developing sensors that can measure levels of critical gases with greater sensitivity and selectivity is of great importance in efforts to reduce the amounts of these gases in certain situations. Sensitivity refers to being able to measure very small amounts of the gases and selectivity refers to being able to detect a particular gas when there are many other gases present. In this project funded by the Office of Integrative Activities (OIA)and the Chemical Structure Dynamics and Mechanisms (CSDM-A) program of the Chemistry Division, Drs. Wang, Riley, and Sunda-Meya are using electrochemical, computational, and microscopy methods to develop new sensors, based on ionic liquids, that can measure gas levels with very high sensitivity and selectivity. An ionic liquid is a room-temperature liquid that, instead of neutral molecules, contains ions (charged molecules). The sensors that are being developed to fit into very small devices and can be used in many different places and applications. In addition to the development of sensors, new methods for investigating the strengths of bonds that hold gas molecules together are being designed. The broader impacts of this work are many, as the newly developed sensors can aid in monitoring, ameliorating, and eliminating gases that are harmful to people and the environment. One of the key features of the project is the direct involvement of undergraduates, giving them opportunities to learn many aspects of research in the physical sciences, organization of data, and preparation/presentation of scientific results and conclusions.This project entails both theoretical and experimental studies aimed at investigating the structures of semiconductor/ionic liquid (SC/IL) interfaces, effective selective adsorption on these interfaces, effects of adsorption on adsorbant bond strength, and understanding of the molecular mechanisms involved therein. This is a fundamental study with strong implications for any future projects involving miniaturized sensors, gas separation, or high-performance catalytic conversion utilizing ILs and/or SCs. This systematic research is being conducted using state-of-the-art electrochemical, spectroscopic, surface science, and computational chemistry methods. The main goals of this project are to achieve a greater fundamental understanding of small molecule adsorption at IL/SC interfaces and to explore new chemistry and physics on these interfaces. ILs generate a very unique solid-like interface; consequently, they can generate extremely high electric fields and induce exceptionally large charge densities at the solid/liquid interface. The electric double layer (EDL) charge density can be much higher than traditional field-effects and allows for new levels of electrostatic modulation to be accessible. The pure ionic structure of IL itself also brings an electrostatic environment, which can potentially be manipulated for facilitating certain small molecule activation. However, electrified IL/electrode interfaces, especially SC's, with adsorbed gas molecules have not been either theoretically or experimentally studied. Here the strong interaction granted by SC with the tunability of IL interfaces are exploited in order to achieve and evaluate gas adsorption that is both sensitive and selective by systematically studying adsorption behavior in the IL environment.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.

小气体分子的检测在工业、环境和其他应用中极其重要。开发能够以更高的灵敏度和选择性测量临界气体水平的传感器对于在某些情况下减少这些气体的量的努力是非常重要的。灵敏度是指能够测量非常少量的气体，选择性是指当存在许多其他气体时能够检测到特定气体。在这个由综合活动办公室（OIA）和化学部的化学结构动力学和机制（CSDM-A）计划资助的项目中，Wang，Riley和Sunda-Meya博士正在使用电化学，计算和显微镜方法开发基于离子液体的新传感器，可以以非常高的灵敏度和选择性测量气体水平。离子液体是一种室温液体，它不是中性分子，而是含有离子（带电分子）。传感器正在开发，以适应非常小的设备，并可用于许多不同的地方和应用。除了传感器的开发，研究将气体分子结合在一起的键强度的新方法也在设计中。这项工作的广泛影响是多方面的，因为新开发的传感器可以帮助监测，改善和消除对人类和环境有害的气体。该项目的主要特点之一是本科生的直接参与，让他们有机会学习物理科学研究的许多方面，数据组织，科学结果和结论的准备/陈述。该项目包括理论和实验研究，旨在研究半导体/离子液体（SC/IL）界面的结构，这些界面上的有效选择性吸附，吸附对吸附剂键强度的影响，以及对其中所涉及的分子机制的理解。这是一项基础性研究，对未来涉及小型化传感器、气体分离或利用离子液体和/或SC的高性能催化转化的任何项目都具有重要意义。这项系统的研究正在使用最先进的电化学，光谱学，表面科学和计算化学方法进行。该项目的主要目标是实现在IL/SC接口的小分子吸附的更大的基本理解，并探索这些接口上的新的化学和物理。离子液体产生非常独特的固体状界面;因此，它们可以产生极高的电场，并在固/液界面处感应出异常大的电荷密度。双电层（EDL）电荷密度可以比传统的场效应高得多，并且允许可访问新水平的静电调制。IL本身的纯离子结构也带来静电环境，其可以潜在地被操纵以促进某些小分子活化。然而，带电IL/电极界面，特别是SC的，与吸附的气体分子还没有被理论或实验研究。在这里，利用SC授予的与IL界面可调性的强相互作用，通过系统地研究IL环境中的吸附行为，实现和评估既敏感又有选择性的气体吸附。该奖项反映了NSF的法定使命，并通过使用基金会的知识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

Sustainable generator and in-situ monitor for reactive oxygen species using photodynamic effect of single-walled carbon nanotubes in ionic liquids

• DOI: 10.1016/j.mtsust.2022.100171
• 发表时间: 2022-07-06
• 期刊: MATERIALS TODAY SUSTAINABILITY
• 影响因子: 7.8
• 作者: Huang，X.;Witherspoon，E.;Dong，P.
• 通讯作者: Dong，P.

Ultra-thin iron phosphate nanosheets for high efficient U(VI) adsorption

超薄磷酸铁纳米片可高效吸附 U(VI)

• DOI: 10.1016/j.jhazmat.2019.02.091
• 发表时间: 2019
• 期刊: Journal of Hazardous Materials
• 影响因子: 13.6
• 作者: De Wang;Yanbin Xu;Difei Xiao;Qingan Qiao;Ping Yin;Zhenglong Yang;Jinxing Li;William Winchester;Zhe Wang;Tasawar Hayat
• 通讯作者: Tasawar Hayat

Ionic Liquids as “Green Solvent and/or Electrolyte” for Energy Interface

• DOI: 10.30919/es8d0013
• 发表时间: 2020-06
• 作者: Zhe Wang;Shu-ang He;V. Nguyen;Kevin E. Riley

Fentanyl Assay Derived from Intermolecular Interaction-Enabled Small Molecule Recognition (iMSR) with Differential Impedance Analysis for Point-of-Care Testing

源自分子间相互作用的小分子识别 (iMSR) 的芬太尼测定以及用于即时测试的差分阻抗分析

• DOI: 10.1021/acs.analchem.2c00017
• 发表时间: 2022
• 期刊: Analytical Chemistry
• 影响因子: 7.4
• 作者: Wang, Zhe;Nautiyal, Amit;Alexopoulos, Christopher;Aqrawi, Rania;Huang, Xiaozhou;Ali, Ashraf;Lawson, Katherine E.;Riley, Kevin;Adamczyk, Andrew J.;Dong, Pei
• 通讯作者: Dong, Pei