Selective transformation of lignocellulose to hydrocarbon chemicals in one reactor

对石油的持续依赖造成了严重的持续问题，包括温室气体排放和供应的地缘政治安全;石油储量减少也导致原油价格上涨，对世界经济产生负面影响。在这种背景下，人们的注意力正转向植物生物量，这是唯一可持续的有机碳来源。来自植物生物质的生物燃料是目前唯一的碳中和、可再生化石燃料替代品。可再生柴油/汽油燃料是未来的运输燃料。 核心研究问题是将高度官能化的糖和木质素衍生的化学品选择性转化为与基础设施相容的脂肪族燃料和芳香族化学品，这些燃料和芳香族化学品与已经从石油中生产的燃料和芳香族化学品相同。本申请中提出的研究解决了这些问题。在一个反应器中，在贫H2条件下实现木质纤维素液化和将分解的中间产物选择性脱氧为烃和化学品。消除加压氢气不仅可以显著降低成本，还可以让分散的小型生物精炼厂使用该技术，因为高压氢气通常可以在集中式工厂获得。用于实现该目标的策略是基于直接脱氧和原位氢气的概念。 本研究的策略性成果为：（1）发展数学模型以定量描述生物质分解过程，类似的研究尚未在文献中记载。(2)定义熔融层并确定分解中间体的催化脱氧机制;（3）了解原位氢气在催化脱氧中的作用;（4）生成耐用的脱氧催化剂;（5）对新的生物质转化工艺进行技术经济评估。 拟议的研究非常适合培养高素质人才（HQP）的新兴就业市场的生物炼制。将培训三名博士生和一名PDF。该发现计划将解决对具有强大工程技能的专家以及新兴生物燃料领域的催化专业知识的未满足需求。

Continued reliance on petroleum oil poses serious ongoing problems that include greenhouse gas emissions and geopolitical security of supply; declining petroleum deposits also lead to rising crude oil prices that negatively impact world economies. Against this background, attention is turning to plant biomass, the only sustainable source of organic carbon. Biofuels derived from plant biomass are currently the only carbon-neutral, renewable alternative to fossil fuels. Renewable diesel/gasoline fuels are the transportation fuels of future. The core research problem is the selective conversion of highly functionalized sugar and lignin-derived chemicals to infrastructure-compatible aliphatic fuels and aromatic chemicals, which are identical to those already produced from petroleum. The research proposed in this application addresses the issues. In one reactor, lignocellulose liquefaction and selective deoxygenation of decomposed intermediates to hydrocarbons and chemicals are realized at lean H2 conditions. Eliminating pressurized hydrogen gas will not only represent significant reduction in costs but also allow decentralized small biorefineries to use the technology, as high pressurized hydrogen gas is often available at centralized plants. The strategies used to achieve the goal are based on the concept of direct deoxygenation and in-situ hydrogen. Strategic outcomes of the proposed research are: (1) Develop mathematical models to quantitatively describe biomass decomposition process; similar research has not been documented in the literature. (2) Define a molten layer and identify the catalytic deoxygenation mechanism of decomposed intermediates; (3) Understand the role of in-situ hydrogen in catalytic deoxygenation (4) Generate a robust, deoxygenation catalyst and (5) Tech-economically evaluate the new biomass conversion process. The proposed research is well suited to train Highly Qualified Personnel (HQP) for the emerging job market on biorefinery. Three PhD students and one PDF will be trained. This Discovery program will address an unmet need for specialists with strong engineering skills as well as catalysis expertise in the emerging area of biofuel.