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找将其直接转化为更高价值碳氢化合物的催化剂和工艺，但这一早期概念探索性研究资助 (EAGER) 项目解决了其中一个问题。这些技术——甲烷氧化偶联 (OCM)——产生了有可能克服商业化障碍的基本见解 OCM 提供了可扩展的技术，可以更有效地利用甲烷，并且净碳排放量比目前更低。技术，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，该项目还包括研究人员机构正在进行的多项教育和外展活动。该项目解决了催化 OCM 技术方面的几个知识差距：1。 ) 缺乏对催化剂（与气相反应相反）如何与反应物偶联以活化甲烷并产生自由基物质的了解，2) 哪种反应模式（多相或气相）控制对所需产物与不需要产物的选择性， 3）将甲烷选择性转化为增值乙烷和乙烯（即 C2）产品的首选催化剂和反应器设计是解决这些挑战的关键。桑迪亚国家实验室用于探测催化剂近表面区域的自由基物质 该仪器以前曾用于纯气相燃烧研究中气相自由基物质的识别（利用。由于缺乏定量研究催化剂和气相物质之间耦合的实验能力，高温 OCM 反应的动力学和机理细节一直未能得到解决。桑迪亚仪器有可能将催化 OCM 的机械和动力学方面提升到新的水平。动力学数据（与表面和气相反应相关）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高转化为 C2 的催化剂和反应器设计GOALI 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，并被认为值得通过以下方式获得支持：评估利用基金会的智力优势和更广泛的影响审查标准。