Collaborative Research: Fundamentals of Natural Gas Conversion to Fuels and Chemicals over Molybdenum Nanostructures

合作研究：通过钼纳米结构将天然气转化为燃料和化学品的基础知识

• 批准号: 1133987
• 负责人: Simon Podkolzin
• 金额: $ 27.6万
• 依托单位: Stevens Institute of Technology
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2011
• 资助国家: 美国
• 起止时间: 2011-11-01 至 2015-04-30
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1133987&HistoricalAwards=false
• 关键词: Collaborative; Research; Fundamentals; Natural; Gas

Natural gas, or methane, is an abundant resource that is unfortunately underutilized due to a lack of efficient technologies that enable its conversion into easily condensable or liquid products amenable to transport. Most natural gas reserves and the associated gas produced in the course of crude oil production at remote locations are classified as stranded, and venting and flaring is a typical method of disposal, resulting in a significant environmental issue as well as a waste of hydrocarbon resource. Natural gas conversion to liquid fuels and chemicals represents a highly desirable goal since North America has some of the largest gas reserves in the world that can serve as a safe and stable source of hydrocarbons. Production of chemicals and liquid fuels from methane is currently dominated by technologies that rely on generation of synthesis gas as the first step. These technologies, however, have an inherent inefficiency since the breaking of all methane C-H bonds in synthesis gas production has to be substantially reversed in subsequent steps. There are, therefore, intense current research efforts for development of direct methods for methane conversion. Research on catalytic methane activation remains an area of high scientific and industrial significance but the catalytic chemistry of methane activation is currently poorly understood. This situation will change with an award made to investigators Simon Podkolzin of the Stevens Institute of Technology, New Jersey, and Israel Wachs of Lehigh University, Pennsylvania. The objective of the proposed research is to develop a molecular level model of catalytic methane conversion to liquid fuels and chemicals by zeolite-supported Mo nanostructures. Methane conversion over Mo nanostructures supported on shape selective zeolites offers a promising alternative for selective methane activation. This chemistry was recently reported by a group from Dalian, China. In this process of methane dehydoaromatization, methane can be converted directly in a single step into benzene with a selectivity of 70-80 mol % and conversions exceeding 10 mol %. In contrast to other direct methane activation chemistries, this process has two unique advantages since methane is converted without any additional reactants. First, complete oxidation of methane to carbon oxides is not possible as in the processes employing O2 or H2O addition. This is also advantageous from the safety perspective. Second, natural gas processing can in concept be performed at remote locations since transportation of reagents is not required. The PIs intend to study the dynamics of active surface sites at the nanoscale under reaction conditions. They will combine the latest developments in molecular spectroscopic characterization techniques (Raman, IR and UV-vis) at the nanoscale under reaction conditions at elevated temperatures with catalyst kinetic testing, kinetic modeling, and quantum-chemical calculations. Advanced time-resolved atomic XANES/EXAFS characterization will be performed in collaboration with Brookhaven National Laboratory. Results of this program will have transformative effects in nanotechnology and energy research by developing nanomaterials for efficient conversion of natural gas into liquid hydrocarbons and potentially making available large reserves of stranded gas, while addressing the environmental issue of venting and burning of associated gas at remote locations. A broad spectrum of educational outreach projects is an integral part of the program, including research experiences as well as university and K-12 teaching modules on energy research and nanomaterials.

天然气或甲烷是一种丰富的资源，不幸的是，由于缺乏有效的技术，使其能够转化为易于冷凝或易于运输的液体产品，因此未得到充分利用。在偏远地区的原油生产过程中产生的大多数天然气储量和伴生气被归类为搁浅，并且排气和燃烧是典型的处置方法，导致严重的环境问题以及烃资源的浪费。天然气转化为液体燃料和化学品是一个非常理想的目标，因为北美拥有世界上最大的天然气储量，可以作为安全和稳定的碳氢化合物来源。从甲烷生产化学品和液体燃料目前主要是依靠合成气作为第一步的技术。然而，这些技术具有固有的低效率，因为在合成气生产中所有甲烷C-H键的断裂必须在随后的步骤中基本上逆转。因此，目前有大量的研究工作用于开发甲烷转化的直接方法。 甲烷催化活化的研究仍然是一个具有高度科学和工业意义的领域，但甲烷活化的催化化学目前知之甚少。随着新泽西史蒂文斯理工学院的西蒙·波德科尔津和宾夕法尼亚州利哈伊大学的伊斯雷尔·瓦克斯的获奖，这种情况将有所改变。该研究的目的是开发分子水平的催化甲烷转化为液体燃料和化学品的沸石负载钼纳米结构的模型。甲烷转化在钼纳米结构上的形状选择性沸石提供了一个有前途的选择性甲烷活化的替代方案。这种化学反应最近由中国大连的一个小组报道。在该方法中，甲烷可以一步直接转化为苯，选择性为70- 80mol%，转化率超过10mol%。与其他直接甲烷活化化学反应相比，该工艺具有两个独特的优势，因为甲烷在没有任何额外反应物的情况下就被转化。首先，甲烷完全氧化成碳氧化物是不可能的，如在使用O2或H2O添加的方法中那样。从安全角度来看，这也是有利的。第二，天然气处理在概念上可以在远程位置进行，因为不需要运输试剂。PI旨在研究反应条件下纳米级活性表面位点的动力学。他们将结合联合收割机的分子光谱表征技术（拉曼，红外和紫外可见光）的最新发展，在纳米级的反应条件下，在高温下与催化剂动力学测试，动力学建模和量子化学计算。 高级时间分辨原子XANES/EXAFS表征将与布鲁克海文国家实验室合作进行。该计划的结果将在纳米技术和能源研究中产生变革性影响，通过开发纳米材料将天然气有效转化为液态烃，并可能提供大量的滞留气体储备，同时解决偏远地区排放和燃烧相关气体的环境问题。广泛的教育推广项目是该计划的一个组成部分，包括研究经验以及关于能源研究和纳米材料的大学和K-12教学模块。