CAREER: Selectivity Control in Methanol-to-Hydrocarbons Catalysis by Manipulating the Hydrocarbon Pool

能源问题显然是21世纪的全球性大挑战。运输燃料是一个重要组成部分，因为目前还没有可行的、世界级规模的碳基燃料替代品。为了满足不断增长的需求，在从石油转向石油的同时，最大限度地提高碳和能源效率，将煤炭、生物质和天然气等碳源转化为这些产品将是至关重要的。在这种转化的所谓C1路线中，碳源与蒸汽和/或氧气反应产生合成气（CO + H2），然后可以反应成一系列产品。甲醇是产生碳氢化合物燃料的产物之一。美国国家科学院2009年的一份题为《煤和生物质液体运输燃料》的报告设想，甲醇制碳氢化合物（MTH）是一个大规模的商业过程，可能会影响未来的运输燃料部门。MTH化学的潜在挑战是进行选择性工作，只生产所需的碳氢化合物产物。美孚公司早在几十年前就将MTG（甲醇制汽油）商业化，从那时起，通过修改所用沸石催化剂的参数，只实现了少量的选择性改变。如何实现更好的碳效率和选择性控制仍然是一个问题。明尼苏达大学双城分校化学工程系的Aditya Bhan教授提出，当我们同时操纵这些反应的催化剂和助催化剂时，将会得到更好的控制。机理研究表明，甲醇的反应是通过烃类池进行的。假设沸石孔是纳米反应器，其中酸位和烃池作为共催化剂。初步数据表明，用其他有机分子作为添加剂来改变碳氢化合物池的性质，确实会显著改变从反应器中出来的产物。Bhan提出了一个实验方案，该方案最终将允许他通过添加各种添加剂来系统地调整MTH的选择性，这些添加剂与适当的沸石催化剂相结合，从而更有效地从C1前体中制造出高辛烷值汽油范围的碳氢化合物，或者轻质聚合物级烯烃。更广泛的影响是，高选择性和原子效率的MTH催化剂系统的发展将导致非石油资源加工的新热化学工艺，以满足对高能量密度和可替代燃料的需求，以解决运输燃料的挑战。这个拟议的项目允许Bhan将化学催化研究与教育和外展组成部分结合起来，强调化学工程在能量转换领域的重要性。通过在能源研究活动中招募和指导来自代表性不足的社区的本科生，以及通过与明尼阿波利斯/圣路易斯市的K-12学校开展课程开发的推广计划，将加强教育。保罗。该奖项是由化学、生物工程、环境和运输系统部门的催化和生物催化项目以及化学部门的化学催化项目联合颁发的。

Energy is clearly a global grand challenge problem for the 21st century. Transportation fuels are a significant component, as there are no viable, world class scale alternatives to carbon-based fuels. To meet the constantly increasing demands while moving from petroleum, it will be essential to maximize carbon and energy efficiency for conversion of carbon sources such as coal, biomass, and natural gas into these products. In the so-called C1 route for this conversion, the carbon sources are reacted with steam and/or oxygen to produce synthesis gas (CO + H2), which can then be reacted to a broad slate of products. Methanol is one of these products which leads to hydrocarbon fuels. A 2009 report by the US National Academies titled Liquid Transportation Fuels from Coal and Biomass envisions methanol-to-hydrocarbons (MTH) as a large-scale commercial process that could impact the transportation fuel sector in the future. The underlying challenge in MTH chemistry is to do a selective job of producing only the hydrocarbon products desired.Mobil has commercialized MTG (methanol-to-gasoline) decades ago, and since then, only minor selectivity modifications have been achieved through modifying the parameters of the zeolite catalyst used. How to achieve better carbon efficiency and selectivity control remains the question. Prof. Aditya Bhan of the Department of Chemical Engineering at the University of Minnesota, Twin Cities proposes that better control will result when we manipulate both the catalyst and co-catalyst for these reactions. Mechanistic studies have shown that the reactions of methanol proceed through a hydrocarbon pool. The hypothesis is that the zeolite pores are nanoreactors in which the acid site and the hydrocarbon pool function as co-catalysts. Preliminary data have demonstrated that changing the nature of the hydrocarbon pool with other organic molecules as additives does significantly change the products coming out of the reactor. Bhan proposes an experimental program which will ultimately allow him to systematically tune selectivity in MTH by the addition of various additives which are combined with the appropriate zeolite catalysts resulting in making higher octane gasoline range hydrocarbons, or alternatively, light polymer grade olefins, more effectively from C1 precursors. The broader impact is the development of highly selective and atom efficient MTH catalyst systems will lead to new thermochemical processes for the processing of non-petroleum resources to meet the demand for high-energy density and fungible fuels to address the transportation fuel challenge. This proposed program allows Bhan to integrate research on chemical catalysis with education and outreach components which highlight the importance of chemical engineering in the area of energy conversion. Education will be enhanced by recruiting and mentoring undergraduate students from under-represented communities in energy research activities, and by an outreach program for curriculum development with K-12 schools in the Minneapolis/St. Paul area. This award is jointly made by the Catalysis and Biocatalysis Program of the Chemical, Bioengineering, Environmental, and Transport Systems Division and the Chemical Catalysis Program of the Division of Chemistry.