CAREER: Selective Thermal Processing of Biomass-derived Oxygenates by Catalytic Fast Pyrolysis

CBET-0747996，Huber智力优点：随着我们的社会远离石油衍生资源，木质纤维素生物燃料将变得越来越重要。木质纤维素生物燃料目前的障碍是缺乏经济的转化方法。理想的工艺是在单个反应器中以短的停留时间从固体生物质选择性地生产液体生物燃料，而无需共同进料氢气。我们最近已经观察到，汽油范围的芳族化合物和烯烃可以在单一反应器中在短停留时间（10-20秒）下以高产率（40%碳产率）由固体生物质衍生的原料生产，而无需在沸石基催化剂上共同进料氢气。这为生物燃料生产引入了一个新的概念，我们称之为催化快速热解。该项目的假设是，芳烃，烷烃和烯烃，所有潜在的生物燃料和生物燃料原料，可以选择性地从热不稳定的生物质衍生的含氧化合物在气相中使用适当的多相催化剂生产。本文主要研究了生物质含氧化合物的催化快速热解反应，主要有三个方面的内容：1）阐明了气相中生物质含氧化合物在多相催化剂上的化学反应途径。这一过程的反应尚未详细研究，我们的首要目标之一是了解与这些反应相关的可能化学途径。我们的原料包括葡萄糖、山梨醇、纤维素和木质素模型化合物。 2)确定催化性能（包括：孔结构，酸碱强度，活性部位的性质）如何改变反应途径。 3)开发研究气相中热不稳定分子转化的方法。生物质衍生的分子通常具有低的热稳定性。为了避免热分解反应，必须使用能够快速加热进料（即500 oC/s）的反应器。我们将在这个项目中测试三个反应器概念：微闪速热解，下流移动床和固定床。这些反应器将允许我们改变加热速率，空速和接触模式。更广泛的影响：该计划将生物燃料研究与教育和推广部分相结合，旨在展示化学工程在生物燃料和可再生能源领域的重要性。虽然人们普遍认为生物学和生物技术对生物燃料至关重要，但催化和化学工程同样重要。我计划通过一系列研讨会，报告和白杨科学讨论，教育科学界，公众，媒体和政策制定者关于催化和化学工程与生物燃料和可再生能源关系的重要性。我还计划通过开发能源技术课程，在化学工程课程中创建能源专业，并将能源概念整合到核心化学工程课程中，将可再生能源融入核心化学工程课程。我帮助在马萨诸塞大学阿默斯特分校建立了一个多学科研究所，专注于生物燃料，其目的是整合研究和教育。我还致力于招募，指导和支持少数民族学生在工程项目通过与东北联盟研究生教育和教授（NEAGEP），这支持努力招募和指导学生从人口群体在科学，技术，工程和数学（干）领域代表不足。拟议的活动将为制定一项综合方案奠定基础，该方案将研究、教育和推广结合起来，重点放在催化和生物燃料上。

CBET-0747996, HuberIntellectual Merit: Lignocellulosic biofuels will become increasingly important as our society moves away from petroleum-derived resources. The current roadblock for lignocellulosic biofuels is the lack of economical conversion processes. The ideal process would selectively produce a liquid biofuel from solid biomass in a single reactor at short-residence times without co-feeding hydrogen. We have recently observed that gasoline range aromatics and olefins can be produced from solid biomass-derived feedstocks in high yields (40 % carbon yield) in a single reactor at short residence times (10-20 s) without co-feeding of hydrogen gas over zeolite based catalysts. This introduces a new concept for biofuel production, which we call catalytic fast pyrolysis. The hypothesis of this project is that aromatics, alkanes and olefins, all potential biofuels and biofuel feedstocks, can selectively be produced from thermally unstable biomass-derived oxygenates in the gas-phase using appropriate heterogeneous catalysts. We will study the catalytic fast pyrolysis of biomass-derive oxygenates with three main objectives: 1) Elucidate the chemical reaction pathways for conversion of biomass-derived oxygenates over heterogeneous catalysts in the gas-phase. The reactions underlying this process have not been studied in detail and one of our first goals is to understand the possible chemical pathways related to these reactions. Our feedstocks include glucose, sorbitol, cellulose and lignin model compounds. 2) Determine how catalytic properties (including: pore structure, acid-base strength, nature of active sites) change the reaction pathway. 3) Develop methods for studying the conversion of thermally unstable molecules in the gas-phase. Biomass-derived molecules generally have a low thermal stability. To avoid thermal decomposition reactions - reactors must be used that allow rapid heating of the feeds (i.e. 500oC/s). We will test three reactor concepts in this project: micro-flash pyrolysis, down-flow moving-bed, and fixed-bed. These reactors will allow us to vary the heating rate, space velocity, and contacting patterns. Broader Impacts: The proposed program integrates research on biofuels with an educational and outreach component that are designed to demonstrate the importance of Chemical Engineering in the area of biofuels and renewable energy. While it is generally accepted that Biology and Biotechnology are vitally important for biofuels it is less well known that Catalysis, and Chemical Engineering are equally important. I plan to educate the scientific community, the general public, media and policy makers on the importance of Catalysis and Chemical Engineering in relationship to biofuels and renewable energy through a series of workshops, reports, and poplar science discussions. I also plan to integrate renewable energy into the core Chemical Engineering curriculum by developing a course on Energy Technology, creating an energy specialization in the Chemical Engineering program, and integrating energy concepts into the core Chemical Engineering curriculum. I have helped establish a multi-disciplinary Institute at UMass-Amherst focused on biofuels whose aim is to integrate research and education. I am also working to recruit, mentor and support minority students in the engineering program by working with Northeast Alliance for Graduate Education and the Professoriate (NEAGEP), which supports efforts to recruit and mentor students from population groups underrepresented in science, technology, engineering, and mathematics (STEM) fields. The proposed activities will provide the foundation on which an integrated program that combines research, education and outreach focusing on catalysis and biofuels will be developed.