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组成部分，尽管长期以来一直在寻求将其直接转换为高价值碳氢化合物的催化剂和过程，但没有一个实现了宽度的工业应用。这项探索性研究（急切）项目的早期概念赠款介绍了其中一种技术 - 甲烷（OCM）的氧化耦合，以产生具有克服商业化障碍的基本见解。 OCM提供可扩展的技术，可更有效地利用甲烷，并且净碳排放量低于当前技术，从而支持美国向可持续能源的过渡，同时确保能源安全。除了技术方面，该项目还包括研究人员机构正在进行的几项教育和外展活动。该项目解决了催化OCM技术中的几个知识差距：1）缺乏对催化剂而不是气相反应的理解，与气相反应相反，与反应物种类的伴侣激活甲烷并产生激进物种，2）哪种反应模式（异质或气相）（异源或气相）控制选择性的选择性，而不是选择的产品，以及优先级别的cat catiesty和Reations的选择性，以及3）乙烯（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。具体而言，研究人员将利用桑迪亚国家实验室的新反应室在催化剂的近表面区域探测激进物种。仪器先前已用于鉴定纯气相混合物研究中气相自由基物种（利用真空 - 硫化光图电离质谱法（VUV-PIMS））。高温OCM反应的动力学和机械细节已经避免了先前的研究者，因为缺乏实验能力，无法定量询问催化剂和气相物种之间的耦合，这与自由基物种的表面产生以及气相中那些物种的后续反应有关。 Sandia仪器有可能将催化OCM的机械和动力学方面提高到新的理解水平。动力学数据（与表面和气相反应相关）将被送入反应堆设计模型（由国家可再生能源实验室（NREL）的合作者开发，以识别催化剂和反应堆设计，这些催化剂和反应堆设计有利于选择性地转化为C2氢碳物种的高度转化为C2氢碳。条件。该奖项反映了NSF的法定使命，并通过使用基金会的知识分子优点和更广泛的影响审查标准评估被认为是宝贵的支持。