EFRI-HyBi: Conversion of Biomass to Fuels using Molecular Sieve Catalysts and Millisecond Contact Time Reactors

研究机构：明尼苏达大学双城分校建议编号：0937706EFRI：EFRI-HYBI：使用分子催化剂和毫秒接触时间反应器将生物质转化为燃料生物质作为碳中性燃料的实际开发需要开发能够处理固体的小型分布式生产系统和克服木质纤维生物质顽固性的化学转化技术。虽然已经提出了几种生物质利用的方法，但没有一种方法能满足商业实施的生产率、可伸缩性、产品分布和经济要求。这项研究的目的是开发一种连续的、可扩展的自热催化过程，在短接触时间的分层反应器中，在金属和沸石基多功能催化剂上将木质纤维生物质“一锅”转化为燃料。这一过程以前从未尝试过，但最近证明了拟议技术的重要元素的可行性，包括：(I)施密特小组在短接触时间自热反应器中从木质纤维颗粒连续无碳生产挥发性有机化合物；(Ii)在纳米水平上控制介孔，以减少沸石催化剂中的传质限制；(Iii)Bhan利用整体支撑的沸石薄膜展示了短接触时间的沸石催化。智力上的优点：生物质生产燃料可以通过将其转化为小碎片，选择性地从碳水化合物中脱氧，以及通过碳-碳键的形成将小中间体转化为大碳氢化合物来实现。建议系统地探索在毫秒接触时间反应器中将生物质的金属放热挥发与沸石脱氧和C-C键形成相结合的可能方法，从而避免有害的多芳烃或固体碳质副产物。为了实现这一变革性的概念，多相催化、反应工程、材料设计和系统集成的新兴前沿将在以下协同研究活动中得到推进：1.Schmidt、Bhan和Vlachos将结合实验和多尺度建模来调整在自热(部分氧化)短接触反应中生物质转化过程中保持碳链长度的产品选择性。TSapatsis将控制沸石基薄膜催化剂的中孔和微孔，以实现毫秒接触时间操作，而Bhan将优化与这些催化剂的脱氧和链生长反应。Floudas将进行计算机筛选，以指导沸石骨架的选择，而Vlachos将开发详细的反应/扩散和微动力学模型。“一锅”反应堆的设计原则将由合作伙伴小组开发和测试。广泛影响：将传统的化学加工和生产转变为可持续的未来是全球社会面临的巨大挑战之一。能够加工木质纤维素原料的小型反应堆系统的开发，将带来利用分散的或目前被浪费的生物质资源的新技术，并有可能为这种转变和美国的经济增长做出贡献。联合绩效指标将把这项工作的内容作为案例研究纳入关于可再生能源和化学品的本科生、研究生和专题课程，以及将在因特网上广泛传播的教学单元。该项目和研究团队的范围和广度进一步为本科生和研究生以及来自代表性不足群体的学生提供了独特的跨学科教育机会。此外，还提出了为中学生开展相关课外活动的外展努力。协理督察致力与公众沟通他们的工作。这将得到大学环境研究所(IonE)提供的基础设施的推动。明尼苏达州大学催化科学与技术中心(CCST)。特拉华州。这项工作的重要发现将包括在IonE和CCST赞助的时事通讯、新闻稿、媒体简报会和公共论坛上。

ABSTRACT PI Name: Michael TsapatsisInstitution: University of Minnesota-Twin CitiesProposal Number: 0937706EFRI: EFRI-HyBi: Conversion of Biomass to Fuels using MolecularSieve Catalysts and Millisecond Contact Time ReactorsThe practical exploitation of biomass as a carbon-neutral source of fuels requires the development of small distributed production systems capable of processing solids and chemical conversion technologies that can overcome the recalcitrance of lignocellulosic biomass. While several processes for biomass utilization have been proposed, none meets the productivity, scalability, product distribution and economic requirements for commercial implementation. The objective of the proposed research is to develop a continuous and scalable autothermal catalytic process for the "one pot" conversion of lignocellulosic biomass to fuels over metal and zeolites based multifunctional catalysts in a short contact time stratified reactor. Such a process has not been attempted before but feasibility of important elements of the proposed technology were recently demonstrated including: (i) the continuous char-free production of volatile organic compounds from lignocellulosic particles in a short contact time autothermal reactor by Schmidt's group; (ii) the control of mesoporosity at the nanometer level to reduce mass transfer limitations in zeolite catalysts by Tsapatsis' group and (iii) the demonstration of short contact time zeolite catalysis by Bhan using monolith supported thin zeolite films.Intellectual Merit: The production of fuels from biomass may be accomplished by its conversion to small fragments, the selective removal of oxygen from carbohydrates, and the conversion of small intermediates into larger hydrocarbons via carbon-carbon bond formation. It is proposed to systematically explore possible ways to combine the metal-based exothermic volatilization of biomass with zeolite-based deoxygenation and C-C bond formation in millisecond contact time reactors thereby avoiding deleterious polyaromatic or solid carbonaceous by-products. To realize this transformative concept, emerging frontiers in heterogeneous catalysis, reaction engineering, material design and systems integration will be advanced in the following synergistic research activities:1. Schmidt, Bhan and Vlachos will combine experiments and multiscale modeling to tune product selectivity towards carbon chain length preservation during biomass conversion in autothermal (partial oxidation) short contact time reactors.2. Tsapatsis will control meso- and microporosity in zeolite-based thin film catalysts to enable millisecond contact time operation and Bhan will optimize deoxygenation and chain growth reactions with these catalysts. Floudas will perform computational screening to guide the selection of zeolites frameworks while detailed reaction/diffusion and microkinetic models will be developed by Vlachos.3. Design principles for the "one pot" reactor will be developed and tested by the team of co-PIs.Broader Impact: Transforming traditional chemical processing and production into a sustainable future is one of the enormous challenges that global society faces. The development of small scale reactor systems capable of processing ligoncellulosic feedstock will lead to new technologies for harnessing diffuse or currently wasted biomass resources and has the potential to contribute to this transformation and the economic growth of the US. The co-PIs will integrate elements of this work as case studies in undergraduate, graduate and topical courses on renewable energy and chemicals, as well as in teaching modules that will be made available on the internet for widespread dissemination. The scope and breadth of the project and the research team further provide unique opportunities for interdisciplinary education of undergraduate and graduate students and students from underrepresented groups. Moreover, an outreach effort to develop related extracurricular activities for middle school students is proposed. The co-PIs are committed in communicating their work to the public. This will be facilitated by the infrastructure provided by the Institute on the Environment (IonE) at the Univ. of Minnesota and the Center for Catalytic Science and Technology (CCST) at the Univ. of Delaware. Important findings from this work will be included in IonE and CCST sponsored newsletters, press releases, media briefings and public forums.