Collaborative Research: ECO-CBET: Methane Conversion by Merging Atmospheric Plasma with Transition-Metal Catalysis

合作研究：ECO-CBET：通过大气等离子体与过渡金属催化相结合进行甲烷转化

基本信息

批准号：
2032604
负责人：
Mark Kushner
金额：
$ 50万
依托单位：
Regents of the University of Michigan - Ann Arbor
依托单位国家：
美国
项目类别：
Continuing Grant
财政年份：
2020
资助国家：
美国
起止时间：
2020-09-01 至 2025-08-31
项目状态：
未结题

来源：
https://www.nsf.gov/awardsearch/showAward?AWD_ID=2032604&HistoricalAwards=false
关键词：
Collaborative Research ECO CBET Methane

项目摘要

Methane is the primary component of natural gas and represents an abundant, alternative chemical feedstock to petroleum. Methane is also a potent greenhouse gas, so excess natural gas from oil fields is flared in order to avoid releasing methane into the atmosphere. Converting natural gas and excess methane into liquid fuels and chemicals would be an efficient way to use natural resources and reduce greenhouse gas emissions. This conversion is challenging, however, when utilizing conventional thermal processes. Low temperature plasma reactor technology is an enticing tool for natural gas methane valorization to fuels and chemicals given its capability to activate hydrocarbons at much lower temperature than thermal processes. Not only does this bring potential to improve rates, but also opens the door to more desirable product selectivity. Despite its allure, practical implementation has been impeded by the complexity of the chemical, physical, and transport processes underlying the technology. This research project studies the valorization of natural gas using catalytic processes conducted in atmospheric plasmas. Little is known about the catalytic conversion of methane in plasmas, so understanding this process could translate into more sustainable chemical routes for methane conversion. The research project will be integrated with educational activities that train students to engineer solutions for sustainable energy, a future without pollution and waste, and reducing greenhouse gas emissions.The research project aims to combine two technologies, plasma-promoted methane activation and transition-metal catalysis, to address methane valorization. The physical properties and chemical reactivity of atmospheric methane plasma are not well understood, nor are subsequent reactions of plasma products with transition metal complexes. Microfluidics techniques will be employed to generate plasmas with controllable properties. Then, experiments will be performed to probe the reactivity of plasmas with organic radical acceptors, to understand how plasmas interact with both organic radical acceptors and organometallic complexes, and to explore carbon-carbon and carbon-nitrogen bond formation in methane plasmas. The ultimate objective is to quantify the reactivity of plasmas with organic radical acceptors and transition metal complexes in order to convert methane into larger alkanes, substituted arenes, and amine compounds. Scale-up and intrinsic energy efficiency present potential challenges to the implementation of plasma-assisted chemical conversion processes. This study will uncover novel approaches for increasing methane reactivity and product selectivity to levels needed for translating fundamental findings into industrial applications.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.

甲烷是天然气的主要成分，是一种丰富的石油替代化学原料。甲烷也是一种强效温室气体，因此油田中多余的天然气会被燃烧，以避免将甲烷释放到大气中。将天然气和多余的甲烷转化为液体燃料和化学品将是利用自然资源和减少温室气体排放的有效方法。然而，当利用传统的热处理工艺时，这种转换具有挑战性。低温等离子体反应器技术是一种将天然气甲烷增值为燃料和化学品的诱人工具，因为它能够在比热处理低得多的温度下激活碳氢化合物。这不仅带来了提高生产率的潜力，而且还为更理想的产品选择性打开了大门。尽管它具有吸引力，但该技术背后的化学、物理和传输过程的复杂性阻碍了实际实施。该研究项目研究利用大气等离子体中进行的催化过程来提高天然气的价值。人们对等离子体中甲烷的催化转化知之甚少，因此了解这一过程可以转化为更可持续的甲烷转化化学路线。该研究项目将与教育活动相结合，培训学生设计可持续能源、没有污染和废物的未来以及减少温室气体排放的解决方案。该研究项目旨在结合两种技术，等离子体促进的甲烷活化和过渡金属催化，解决甲烷增值问题。大气甲烷等离子体的物理性质和化学反应性以及等离子体产物与过渡金属络合物的后续反应尚不清楚。将采用微流体技术来产生具有可控特性的等离子体。然后，将进行实验来探测等离子体与有机自由基受体的反应性，了解等离子体如何与有机自由基受体和有机金属配合物相互作用，并探索甲烷等离子体中碳-碳和碳-氮键的形成。最终目标是量化等离子体与有机自由基受体和过渡金属络合物的反应性，以便将甲烷转化为更大的烷烃、取代的芳烃和胺化合物。规模化和内在能源效率对等离子体辅助化学转化工艺的实施提出了潜在的挑战。这项研究将揭示提高甲烷反应性和产品选择性至将基本发现转化为工业应用所需水平的新方法。该奖项反映了 NSF 的法定使命，并通过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，被认为值得支持。

项目成果

期刊论文数量（6）

专著数量（0）

科研奖励数量（0）

会议论文数量（0）

专利数量（0）

HCOO − aq degradation in droplets by OH aq in an atmospheric pressure glow discharge

HCOO → OH aq 在大气压辉光放电中对液滴的降解

DOI：
10.1088/1361-6463/acc958
发表时间：
2023-04
期刊：
Journal of Physics D: Applied Physics
影响因子：
0
作者：
Meyer, Mackenzie;Nayak, Gaurav;Bruggeman, Peter J.;Kushner, Mark J.
通讯作者：
Kushner, Mark J.

A surface mechanism for O 3 production with N 2 addition in dielectric barrier discharges

介质阻挡放电中添加 N 2 产生 O 3 的表面机制

DOI：
10.1088/1361-6595/ace95d
发表时间：
2023-08
期刊：
Plasma Sources Science and Technology
影响因子：
3.8
作者：
Meyer, Mackenzie;Foster, John;Kushner, Mark J.
通讯作者：
Kushner, Mark J.

Atmospheric pressure plasma treatment of skin: penetration into hair follicles

常压等离子皮肤治疗：渗透到毛囊

DOI：
10.1088/1361-6595/acef59
发表时间：
2023-08
期刊：
Plasma Sources Science and Technology
影响因子：
3.8
作者：
Konina, Kseniia;Freeman, Theresa A.;Kushner, Mark J.
通讯作者：
Kushner, Mark J.

The 2022 Plasma Roadmap: low temperature plasma science and technology

2022年等离子体路线图：低温等离子体科学与技术

DOI：
10.1088/1361-6463/ac5e1c
发表时间：
2022-07
期刊：
Journal of Physics D: Applied Physics
影响因子：
0
作者：
Adamovich, I;Agarwal, S;Ahedo, E;Alves, L L;Baalrud, S;Babaeva, N;Bogaerts, A;Bourdon, A;Bruggeman, P J;Canal, C;et al
通讯作者：
et al

Reaction mechanism for atmospheric pressure plasma treatment of cysteine in solution

常压等离子体处理溶液中半胱氨酸的反应机理

DOI：
10.1088/1361-6463/ace196
发表时间：
2023-07
期刊：
Journal of Physics D: Applied Physics
影响因子：
0
作者：
Polito, Jordyn;Herrera Quesada, María J.;Stapelmann, Katharina;Kushner, Mark J.
通讯作者：
Kushner, Mark J.