QLC: EAGER: Study of the hydrocarbon quantum formation process with carbon 12 and carbon 13 and optical control

QLC：EAGER：碳12和碳13碳氢化合物量子形成过程及光控制研究

• 批准号: 1836540
• 负责人: Mengyan Shen
• 金额: $ 12.37万
• 依托单位: University of Massachusetts Lowell
• 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 2020-08-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1836540&HistoricalAwards=false
• 关键词: QLC; EAGER; Study; hydrocarbon; quantum

In this project, funded by the Chemical Structure, Dynamic & Mechanism B Program of the Chemistry Division, Professor Mengyan Shen at University of Massachusetts Lowell (UML) is testing the hypothesis that chain hydrocarbons are quantum mechanically synthesized on a cobalt/cobalt oxide surface from carbon dioxide, water, and light. This reaction mimics photosynthesis and is important in reducing carbon dioxide and increasing the energy supply. The goals of this research are to exploit the characteristics of an unusual isotope distribution that is completely different from conventional expectation. The project provides great opportunities for training students including those underrepresented in sciences. It also helps to develop a workforce on quantum computing. Outreach activities involving K-12 students will also be part of the funded project. A cobalt oxide photo-catalyst, discovered in Professor Shen's lab at UML, is physically activated by sunlight and has been proven to directly convert carbon dioxide and water to long-chain hydrocarbons (C5 to C15). When a mixture of isotopic C-12 and C-13 carbon dioxide was used, a highly unusual isotope distribution was observed. Particular objectives of this proposal are (1) To confirm the observation that pure C-12 hydrocarbons and pure C-13 hydrocarbons tend to form easily on some catalysts' surfaces, which cannot be explained with the current chemical theories, (2) To understand and create a predictive model for the mechanism of the formation of chain hydrocarbons based on experimental results using isotopic carbon dioxide and isotopic water. It is hoped that this would explain the observation of pure C-13 and pure C-12 having the tendency to group together in forming chain hydrocarbons, and (3) To find controlling parameters with light wavelength, temperature, and pressures as well as study the influence of the catalyst surface structures on the quantum formation of hydrocarbons.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.

在这项由化学系化学结构、动力学和机理B计划资助的项目中，马萨诸塞大学洛厄尔分校的沈梦燕教授正在验证一种假设，即链烃是由二氧化碳、水和光在钴/钴氧化物表面通过量子力学合成的。这种反应模拟光合作用，在减少二氧化碳和增加能源供应方面很重要。这项研究的目的是探索一种与传统预期完全不同的不同寻常的同位素分布的特征。该项目为培训学生提供了很好的机会，包括那些在科学领域代表性不足的学生。它还有助于发展一支量子计算的劳动力队伍。涉及K-12学生的外展活动也将是该资助项目的一部分。在哈佛大学沈教授的实验室中发现了一种氧化钴光催化剂，它被阳光物理激活，并已被证明可以直接将二氧化碳和水转化为长链碳氢化合物(C5至C15)。当使用同位素C-12和C-13二氧化碳的混合物时，观察到一种非常不寻常的同位素分布。这一建议的具体目标是：(1)证实纯C-12烃和纯C-13烃倾向于在某些催化剂表面容易形成的观察结果，这是目前的化学理论无法解释的；(2)根据使用同位素二氧化碳和同位素水的实验结果，理解并建立链烃形成机理的预测模型。希望这将解释观察到的纯C-13和纯C-12在形成链烃时有聚集在一起的趋势，以及(3)寻找与光波长、温度和压力有关的控制参数，以及研究催化剂表面结构对烃类量子形成的影响。这一奖项反映了NSF的法定使命，并通过使用基金会的智力优势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

Conversion of water and carbon dioxide into methanol with solar energy on Au/Co nanostructured surfaces

• DOI: 10.1088/2053-1591/ab7d0e
• 发表时间: 2020-03-01
• 期刊: MATERIALS RESEARCH EXPRESS
• 影响因子: 2.3
• 作者: Zhu, Qinghua;Wang, Cong;Shen, Mengyan
• 通讯作者: Shen, Mengyan

Low-cost visible-light photosynthesis of water and adsorbed carbon dioxide into long-chain hydrocarbons

• DOI: 10.1016/j.cplett.2019.136985
• 发表时间: 2020-01-01
• 期刊: CHEMICAL PHYSICS LETTERS
• 影响因子: 2.8
• 作者: Wang, Cong;Ren, Haizhou;Mazur, Eric
• 通讯作者: Mazur, Eric

Carbon isotope effects in the artificial photosynthesis reactions catalyzed by nanostructured Co/CoO

纳米结构Co/CoO催化的人工光合作用反应中的碳同位素效应

• DOI: 10.1016/j.cplett.2020.137731
• 发表时间: 2020
• 期刊: Chemical Physics Letters
• 影响因子: 2.8
• 作者: Zeng, Ming;Kan, Zhe;Wang, Zibo;Shen, Mengyan
• 通讯作者: Shen, Mengyan