EAGER: GOALI: Explicating the gas-surface coupled reaction in oxidative coupling of methane via reaction kinetics, operando spectroscopy, photoionization spectrometry

渴望：目标：通过反应动力学、操作光谱、光电离光谱法解释甲烷氧化偶联中的气体-表面偶联反应

• 批准号: 2327344
• 负责人: Jonas Baltrusaitis
• 金额: $ 30万
• 依托单位: Lehigh University
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2023
• 资助国家: 美国
• 起止时间: 2023-07-01 至 2025-06-30
• 项目状态: 未结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=2327344&HistoricalAwards=false
• 关键词: EAGER; GOALI; Explicating; gas; surface

Methane is the major component of natural gas, and while catalysts and processes that convert it directly to higher-value hydrocarbons have long been sought, none have achieved widespread industrial application. This Early-concept Grant for Exploratory Research (EAGER) project addresses one of those technologies – Oxidative Coupling of Methane (OCM) – to generate fundamental insights that have potential to overcome barriers to commercialization. OCM offers scalable technology that would utilize methane more efficiently, and with lower net carbon emissions than current technology, thus supporting the U.S. transition to sustainable energy, while ensuring energy security. Beyond the technical aspects, the project includes several on-going educational and outreach activities at the investigators’ institution. The project addresses several knowledge gaps in catalytic OCM technology: 1) lack of understanding of how the catalyst, as opposed to the gas phase reactions, couples with the reactant species to activate methane and generate radical species, 2) which reaction mode (heterogeneous or gas phase) controls selectivity to desired versus undesired products, and 3) what are preferred catalyst and reactor designs for converting methane selectively to value-added ethane and ethylene (i.e., C2) products. Collaboration with scientists at Sandia National Labs is key to addressing those challenges. Specifically, the investigators will utilize a novel reaction chamber at Sandia National Labs for probing radical species in the near-surface region of a catalyst. The instrumentation has previously been used for identification of gas phase radical species in pure gas phase combustion studies (utilizing vacuum-ultraviolet photoionization mass spectrometry (VUV-PIMS)). Kinetic and mechanistic details of the high-temperature OCM reaction have eluded prior investigators because of lack of experimental capability to quantitatively interrogate the coupling between the catalyst and gas phase species as related to the surface generation of radical species and subsequent reaction of those species in the gas phase. The Sandia instrumentation has the potential to take mechanistic and kinetic aspects of catalyzed OCM to new levels of understanding. The kinetic data (as related to both surface and gas-phase reactions) will be fed into reactor design models (developed by a collaborator at the National Renewable Energy Laboratory (NREL) to identify catalyst and reactor designs that favor high conversion of methane selectively to C2 hydrocarbon species. In a separate thrust the GOALI partner PCI, Inc will conduct a thousand-hour durability evaluation of the state-of-the-art catalyst under industrial operating conditions.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，虽然长期以来一直在寻求将其直接转化为更高价值的碳氢化合物的催化剂和工艺，但没有一种实现了广泛的工业应用。 这个早期概念探索性研究资助（EAGER）项目涉及其中一项技术-甲烷氧化偶联（OCM）-以产生有可能克服商业化障碍的基本见解。 OCM提供可扩展的技术，可以更有效地利用甲烷，并且比当前技术的净碳排放量更低，从而支持美国向可持续能源转型，同时确保能源安全。 除技术方面外，该项目还包括在调查机构开展的若干持续教育和外联活动。该项目解决了催化OCM技术中的几个知识空白：1）缺乏对与气相反应相反的催化剂如何与反应物物质偶联以活化甲烷并产生自由基物质的理解，2）哪种反应模式（非均相或气相）控制对所需产物和不需要产物的选择性，和3）用于将甲烷选择性转化为增值的乙烷和乙烯的优选催化剂和反应器设计是什么（即，C2）产品。 与桑迪亚国家实验室的科学家合作是应对这些挑战的关键。 具体来说，研究人员将利用桑迪亚国家实验室的一种新型反应室来探测催化剂近表面区域的自由基物种。该仪器以前已被用于识别气相自由基物种在纯气相燃烧研究（利用真空紫外光电离质谱法（VUV-PIMS））。 高温OCM反应的动力学和机理细节已经回避了先前的研究者，因为缺乏实验能力来定量询问催化剂和气相物质之间的耦合，如与自由基物质的表面生成和这些物质在气相中的后续反应有关。桑迪亚仪器有可能采取催化OCM的机制和动力学方面的理解到新的水平。动力学数据（与表面和气相反应有关）将被输入反应器设计模型（由国家可再生能源实验室（NREL）的合作者开发，以确定有利于甲烷选择性地高转化为C2烃类的催化剂和反应器设计。 GOALI的合作伙伴PCI，Inc将在工业操作条件下对最先进的催化剂进行千小时耐久性评估。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。