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

名称：Michael tsapatsi机构：明尼苏达大学双城分校提案号：0937706EFRI: EFRI-HyBi：利用分子筛催化剂和微差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来源的实际开发需要开发能够处理固体和化学转化技术的小型分布式生产系统，这些系统可以克服木质纤维素生物质的难阻性。虽然提出了几种生物质的利用方法，但没有一种方法符合商业实施的生产力、可扩展性、产品分配和经济要求。提出的研究目标是开发一种连续和可扩展的自热催化过程，用于在短接触时间分层反应器中将木质纤维素生物质转化为基于金属和沸石的多功能催化剂的“一锅”燃料。以前从未尝试过这种工艺，但最近证明了所提出技术的重要组成部分的可行性，包括：(i) Schmidt的小组在短接触时间自热反应器中从木质纤维素颗粒连续无炭生产挥发性有机化合物；（ii） Tsapatsis小组在纳米水平上控制介孔，以减少沸石催化剂的传质限制；（iii） Bhan使用整体支撑的沸石薄膜进行短接触时间沸石催化的演示。智力优势：从生物质中生产燃料可以通过将其转化为小碎片，从碳水化合物中选择性去除氧，以及通过碳-碳键形成将小中间体转化为较大的碳氢化合物来完成。建议系统探索在毫秒接触时间反应器中将生物质的金属基放热挥发与沸石基脱氧和C-C键形成结合起来的可能方法，从而避免有害的多芳族或固体碳质副产物。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：Schmidt， Bhan和Vlachos将结合实验和多尺度建模来调整自热（部分氧化）短接触时间反应器中生物质转化过程中碳链长度保存的产品选择性。Tsapatsis将控制沸石基薄膜催化剂的介孔和微孔，以实现毫秒级的接触时间操作，Bhan将优化这些催化剂的脱氧和链生长反应。fludas将进行计算筛选，以指导分子筛框架的选择，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项目负责人团队开发和测试。更广泛的影响：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。能够处理木质纤维素原料的小型反应器系统的发展将导致利用分散或目前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。这些合作项目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、研究生课程和专题课程，并纳入将在互联网上广泛传播的教学模块。项目的范围和广度以及研究团队进一步为本科生和研究生以及来自弱势群体的学生提供了跨学科教育的独特机会。此外，还提出了拓展中学生课外活动的建议。共同调查专员致力向公众传达他们的工作。明尼苏达大学环境研究所（IonE）和特拉华大学催化科学与技术中心（CCST）提供的基础设施将为这项工作提供便利。这项工作的重要发现将包括在IonE和CCST赞助的通讯、新闻稿、媒体简报和公共论坛中。

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.