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CAS: Photochemical CO2 Reduction Using Biomimetic NAD+/NADH Analogs

CAS：使用仿生 NAD /NADH 类似物进行光化学 CO2 还原

基本信息

批准号：
1954298
负责人：
Ksenija Glusac
金额：
$ 49万
依托单位：
University of Illinois at Chicago
依托单位国家：
美国
项目类别：
Standard Grant
财政年份：
2020
资助国家：
美国
起止时间：
2020-08-01 至 2024-07-31
项目状态：
已结题

来源：
https://www.nsf.gov/awardsearch/showAward?AWD_ID=1954298&HistoricalAwards=false
关键词：
CAS Photochemical CO2 Reduction Using

项目摘要

With this award, the Chemical Catalysis Program in the Division of Chemistry is funding Dr. Ksenija Glusac of the University of Illinois-Chicago to develop carbon dioxide-reduction chemistry through an approach inspired from nature, particularly from photosynthesis through which plants use sunlight to convert CO2 into useful carbohydrates. This project explores ways in which energy from the sun can be utilized to meet our energy demand. The Glusac research group aims to convert carbon dioxide to methanol, a liquid fuel that can be easily transported and handled. The main challenge in this project is that, in addition to methanol, many other products can be formed from carbon dioxide. Dr. Glusac is exploring catalysts to perform the desired chemical reaction selectively to form methanol with high efficiency. These catalysts are being made from earth-abundant elements, with the aim of enabling their widespread use in future devices. The catalyst needs to absorb light emitted by the sun and then use the absorbed energy to perform useful chemistry. Catalyst/semiconductor hybrid materials that can absorb sunlight and use the absorbed energy for the desired conversion of carbon dioxide to methanol are being investigated. As part of this project, Dr. Glusac is also developing online educational materials for students and general population in the area of photochemistry, a branch of chemistry that investigates how light interacts with molecules. Inspired by natural photosynthesis, Dr. Ksenija Glusac of the University of Illinois-Chicago is investigating photocatalytic CO2 reduction by metal-free NADH analogs that are photogenerated from NAD+ analogs using water as an electron and proton source. The main hypothesis of this project is that, using a proposed hydride transfer mechanism, the CO2 reduction can be selectively directed toward methanol production. The research thrusts are grouped into two sections: one addressing the “dark” portion of catalysis, namely the reduction of CO2 by organic hydrides, and the second exploring the closure of the catalytic cycle via photochemical regeneration of those hydrides. The experimental approach involves studying the thermodynamic hydricities of organic hydrides and investigating the kinetics of hydride transfer to either CO2 or an activated form of CO2. The Glusac team is developing systems to effect thermal CO2 hydrogenation using a combination of NAD+ (nicotinamide adenine dinucleotide) analogues and Lewis bases, with electrochemical regeneration of organic hydrides using a proton-coupled approach, and photochemical regeneration of organic hydrides using mid- and wide-gap semiconductors. This study is providing new mechanisms for coupling thermodynamically uphill reduction processes with visible light energy. Dr. Glusac's educational activities involve the development of online lecture materials in the area of photochemistry. These video lectures are enabling the dissemination of knowledge to students and the general population interested in the fundamentals and applications of photochemistry.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.

有了这个奖项，化学系的化学催化项目资助伊利诺伊大学芝加哥分校的Ksenija Glusac博士通过一种受自然启发的方法开发二氧化碳还原化学，特别是通过光合作用，植物利用阳光将二氧化碳转化为有用的碳水化合物。这个项目探索了如何利用太阳能来满足我们的能源需求。Glusac研究小组的目标是将二氧化碳转化为甲醇，这是一种易于运输和处理的液体燃料。该项目的主要挑战是，除了甲醇，许多其他产品可以由二氧化碳形成。Glusac博士正在探索催化剂，以选择性地进行所需的化学反应，从而高效地形成甲醇。这些催化剂是由地球上丰富的元素制成的，目的是使它们能够在未来的设备中广泛使用。催化剂需要吸收太阳发出的光，然后利用吸收的能量进行有用的化学反应。催化剂/半导体混合材料可以吸收太阳光，并使用所吸收的能量的二氧化碳到甲醇的所需的转换正在研究中。作为该项目的一部分，Glusac博士还在为学生和普通人群开发光化学领域的在线教育材料，光化学是化学的一个分支，研究光如何与分子相互作用。受自然光合作用的启发，伊利诺伊大学芝加哥分校的Ksenija Glusac博士正在研究通过无金属的NADH类似物进行光催化CO2还原，这些类似物是使用水作为电子和质子源从NAD+类似物中光生的。该项目的主要假设是，使用所提出的氢化物转移机制，可以选择性地将CO2还原导向甲醇生产。研究重点分为两个部分：一个是解决催化的“黑暗”部分，即通过有机物还原CO2，第二个是探索通过这些有机物的光化学再生关闭催化循环。实验方法包括研究有机氢化物的热力学氢化度，并研究氢化物转移到CO2或活化形式的CO2的动力学。Glusac团队正在开发使用NAD+（烟酰胺腺嘌呤二核苷酸）类似物和刘易斯碱的组合来实现热CO2氢化的系统，使用质子耦合方法进行有机物的电化学再生，以及使用中隙和宽隙半导体进行有机物的光化学再生。这项研究为化学上坡还原过程与可见光能量的耦合提供了新的机制。Glusac博士的教育活动涉及光化学领域的在线讲座材料的开发。这些视频讲座使知识传播到学生和普通大众感兴趣的基础和应用的光化学。这个奖项反映了NSF的法定使命，并已被认为是值得通过评估使用基金会的知识价值和更广泛的影响审查标准的支持。

项目成果

期刊论文数量（11）

专著数量（0）

科研奖励数量（0）

会议论文数量（0）

专利数量（0）

Proton-Coupled Electron Transfer in a Ruthenium(II) Bipyrimidine Complex in Its Ground and Excited Electronic States

处于基态和激发电子态的钌(II)联嘧啶络合物中的质子耦合电子转移

DOI：
10.1021/acs.jpca.2c02255
发表时间：
2022
期刊：
The Journal of Physical Chemistry A
影响因子：
0
作者：
Drummer, Matthew C.;Weerasooriya, Ravindra B.;Gupta, Nikita;Askins, Erik J.;Liu, Xiaolin;Valentine, Andrew J.;Li, Xiaosong;Glusac, Ksenija D.
通讯作者：
Glusac, Ksenija D.

Strong Electronic Coupling of Graphene Nanoribbons onto Basal Plane of a Glassy Carbon Electrode

石墨烯纳米带在玻碳电极基面上的强电子耦合

DOI：
10.1021/acsaelm.0c00978
发表时间：
2021
期刊：
ACS Applied Electronic Materials
影响因子：
4.7
作者：
Zoric, Marija R.;Askins, Erik J.;Qiao, Xiaoxiao;Glusac, Ksenija D.
通讯作者：
Glusac, Ksenija D.

Ultrafast Laser Pulse Generation by Mode Locking: Matlab-based Demonstrations

通过锁模生成超快激光脉冲：基于 Matlab 的演示

DOI：
发表时间：
2022
期刊：
ChemRxiv
影响因子：
0
作者：
Aleksei Goun;Ksenija Glusac
通讯作者：
Ksenija Glusac

Kinetics of Hydride Transfer from Catalytic Metal-Free Hydride Donors to CO 2

氢化物从催化无金属氢化物供体向CO 2 转移的动力学

DOI：
10.1021/acs.jpclett.0c03662
发表时间：
2021
期刊：
The Journal of Physical Chemistry Letters
影响因子：
0
作者：
Weerasooriya, Ravindra B.;Gesiorski, Jonathan L.;Alherz, Abdulaziz;Ilic, Stefan;Hargenrader, George N.;Musgrave, Charles B.;Glusac, Ksenija D.
通讯作者：
Glusac, Ksenija D.

Long-Lived Excited State in a Solubilized Graphene Nanoribbon