EAGER: Selectivity Control in Direct Non-oxidative Methane Conversion over Fe?SiO2 Catalyst by Manipulating the Feed Composition

该项目是一项探索性研究，旨在确认和扩展发表在《科学》杂志上的一份报告（Guo等人，2014年），该报告涉及一种铁-二氧化硅催化剂和反应条件，可将甲烷直接非氧化转化（DNMC）为更高价值的化学原料，包括乙烯、苯和萘。 该技术如果得到证实，将是一项重大的技术突破，具有将大量页岩气衍生甲烷转化为可运输的高价值化学原料的变革潜力，而不是目前的燃烧做法，伴随着温室气体的排放，甲烷化学中的潜在挑战是以经济的方法进行活性和选择性催化转化以形成燃料和化学品而不会通过热处理或焦炭形成使催化剂失活。PI将通过催化剂精细结构的非原位分析和使用分子束质谱（MBMS）分析稳定和自由基气相反应中间体和产物来阐明在Fe©SiO2催化剂上的DNMC反应中的反应途径和机理。该研究还将评估氢气和烃类物质对催化的影响，作为控制DNMC的参数，并证明其在以下特定目标背景下的适用性：（i）成功合成催化剂并了解其活化机制;（ii）通过控制进料流组成系统地调节产物选择性和甲烷转化率;（iii）严格描述进料组成对甲烷反应途径和催化剂失活的动力学影响。拟议的研究将为开发催化剂和工艺提供具体指导，这些催化剂和工艺可用于从低成本甲烷气体资源中制造增值产品。 为此，实际DNMC过程的更广泛影响将改变燃料和化学品行业，同时减少大气中的二氧化碳负担和化石资源对全球变暖的影响。该技术还可能应用于其他领域，如处理来自生物可再生来源的热解气体。该研究将为研究生和本科生创造一个独特的机会，体验催化，反应工程，气体分析和化学动力学方面的交叉教育。该奖项由新兴前沿和多学科活动工程理事会办公室共同资助。

The project is an exploratory study aimed at confirming and extending a report published in Science (Guo et al. 2014) of an iron-silica catalyst and reaction conditions leading to direct, non-oxidative, methane conversion (DNMC) to higher-value chemical feedstocks including ethylene, benzene, and naphthalene. The technology, if proven, represents a significant technological breakthrough with transformative potential for converting the large quantities of shale gas derived methane to transportable, high-value chemical feedstocks rather than the current practice of flaring with associated emissions of the greenhouse gas, carbon dioxide.The underlying challenge in methane chemistry is active and selective catalytic conversion to form fuels and chemicals in an economical approach without deactivating the catalyst via thermal processes or coke formation. The PIs will elucidate the reaction pathways and mechanisms in the DNMC reactions over Fe©SiO2 catalyst by ex-situ analysis of catalyst fine structures and using Molecular Beam Mass Spectroscopy (MBMS)to analyze both stable and radical gas phase reaction intermediates and products. The study will also evaluate the effects of hydrogen and hydrocarbon species on catalysis as a parameter to control DNMC and demonstrate its applicability in context of the following specific aims: (i) Successfully synthesize the catalyst and understand its activation mechanism; (ii) Systematically tune the product selectivity and methane conversion by controlling the feed stream compositions; (iii) Rigorously describe the kinetic effects of feed composition on methane reaction pathways and catalyst deactivation. The proposed research will provide specific guidance for the development of catalysts and processes useful in manufacturing value-added products from low cost methane gas resources. To this end the broader impact of a practical DNMC process would transform the fuels and chemicals industry while reducing the atmospheric burden of CO2 and the impact of fossil resources on global warming. The technology could also have potential application in other areas such as processing of pyrolysis gases from biorenewable sources. The study will create a unique opportunity for graduate and undergraduate students to experience cross-cutting education in aspects of catalysis, reaction engineering, gas analysis, and chemical kinetics.This award is co-funded by the Engineering Directorate Office of Emerging Frontiers and Multidisciplinary Activities.