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

甲烷是天然气的主要成分，是石油的一种丰富的替代化学原料。甲烷也是一种强效的温室气体，因此为了避免将甲烷释放到大气中，多余的油田天然气被燃烧。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途径。然而，当利用传统的热过程时，这种转换是具有挑战性的。低温等离子体反应器技术是天然气甲烷转化为燃料和化学品的诱人工具，因为它能够在比热过程低得多的温度下激活碳氢化合物。这不仅带来了提高利率的潜力，而且还为更理想的产品选择性打开了大门。尽管它很有吸引力，但实际实施一直受到技术基础的化学、物理和运输过程的复杂性的阻碍。本研究项目研究天然气在大气等离子体中催化过程的增值。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为甲烷转化提供更可持续的化学途径。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、没有污染和浪费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等离子体促进甲烷活化和过渡金属催化两种技术来解决甲烷增值问题。大气甲烷等离子体的物理性质和化学反应性尚不清楚，等离子体产物与过渡金属配合物的后续反应也不清楚。微流体技术将用于产生具有可控特性的等离子体。接下来，我们将通过实验探索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。最终目的是量化等离子体与有机自由基受体和过渡金属配合物的反应性，以便将甲烷转化为更大的烷烃、取代芳烃和胺化合物。放大和内在能量效率是等离子体辅助化学转化过程实施的潜在挑战。这项研究将发现提高甲烷反应性和产品选择性的新方法，使其达到将基础发现转化为工业应用所需的水平。该奖项反映了美国国家科学基金会的法定使命，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。

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.