Collaborative Research: Experimental and computational methods to study chemical transformations of solid xylose into useful compounds

合作研究：研究固体木糖化学转化为有用化合物的实验和计算方法

• 批准号: 1703638
• 负责人: Jim Pfaendtner
• 金额: $ 22.5万
• 依托单位: University of Washington
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2017
• 资助国家: 美国
• 起止时间: 2017-09-01 至 2021-11-30
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1703638&HistoricalAwards=false
• 关键词: Collaborative; Research; Experimental; computational; methods

The long-term security of our economy requires a portfolio of domestic feedstocks to produce fuels and chemicals. Biomass is a promising choice; however, conversion technologies that are reliable, reproducible and economical have yet to come to market. Because of its low cost and versatility, biomass fast pyrolysis technology is an ideal choice for producing a renewable stream of fuels and chemicals. One issue with this technology that limits its implementation is that the underlying physical and chemical properties of the biomass transformations remain largely unknown. This project is a collaborative research study involving engineering groups at the Universities of Minnesota and Washington. In parallel, the teams are carrying out a detailed fundamental investigation using experimental (Minnesota) and computational (Washington) methods. The research has the overall goal of determining the mechanism of the chemical transformation of xylan, a major constituent of renewable biomass, into small molecule compounds that are precursors for fuels and chemicals. The research will also benefit other high temperature conversions of similar feedstocks to form a wide product slate. The educational benefits of this project are impacting graduate and undergraduate researchers. The collaborative project mechanism is an ideal way to enrich the training of students who specialize in experimental or theoretical methods through regular interactions and joint publication of research. The outcomes of this research project will also enrich chemical engineering coursework by the addition of real world problems and mini-projects stemming from the research results. The objective of this fundamental research project is to elucidate all of the key pyrolysis reaction pathways in the evolution of xylan, a biopolymer, to products. The experimental effort is based a new technique called PHASR (Pulsed heated analysis of solid reactions), that is capable of measuring rates of conversion in a regime totally free from transport limitations. The simulations and modeling combine graph theory, ab initio dynamics with the metadynamics method, and kinetic Monte Carlo modeling. The team is first investigating the physics of forming a liquid intermediate phase and the properties of the liquid intermediate with experiments and simulations. After determining the structure and dynamics of the transient intermediate, the project will focus on the kinetics and mechanism of biomass conversion. Detailed PHASR analysis is combined with graph theory to determine suggestions for how intermediate and final small molecule products are formed. Building on this, ab initio molecular dynamics (MD) and cutting edge methods developed by the researchers are used to discover individual reaction pathways and characterize their rates. The final step combines the experiments and new mechanistic insights to build a detailed overall model capable of describing both the overall physics and chemistry of this process.

我们经济的长期安全要求国内原料组合生产燃料和化学物质。生物质是一个有前途的选择；但是，可靠，可重复和经济的转换技术尚未推向市场。由于其成本低和多功能性，生物质快速热解技术是生产可再生燃料和化学物质流的理想选择。这项限制其实施的技术的一个问题是，生物质转化的基本物理和化学特性在很大程度上尚不清楚。该项目是一项合作研究，涉及明尼苏达州和华盛顿大学的工程小组。同时，这些团队正在使用实验（明尼苏达州）和计算（华盛顿）方法进行详细的基本调查。这项研究的总体目标是确定可再生生物量的主要成分木聚体的化学转化机制，成为小分子化合物，这些化合物是燃料和化学物质的前体。这项研究还将受益于类似原料的其他高温转化，形成广泛的产品板岩。该项目的教育益处正在影响研究生和本科研究人员。协作项目机制是通过定期互动和共同出版研究来丰富专门从事实验或理论方法的学生培训的理想方式。该研究项目的结果还将通过增加现实世界中的问题和研究结果所引起的迷你项目来丰富化学工程课程。这个基本研究项目的目的是阐明生物聚合物Xylan进化中的所有关键热解反应途径。实验性工作是基于一种称为PHASR的新技术（对固体反应的脉冲加热分析），该技术能够在完全没有运输限制的情况下衡量转化率。仿真和建模将图理论，从头算动力学与元动力学方法和动力学蒙特卡洛建模相结合。该团队首先研究形成液体中间相的物理学以及通过实验和仿真的液体中间体的特性。在确定了瞬态中间体的结构和动力学之后，该项目将集中于生物量转化的动力学和机理。详细的PHASR分析与图理论相结合，以确定有关中间和最终小分子产物的建议。以此为基础，研究人员开发的Ab Inli算分子动力学（MD）和尖端方法被用来发现单个反应途径并表征其速率。最后一步结合了实验和新的机械见解，以建立一个详细的总体模型，能够描述该过程的整体物理和化学。

项目成果

Deconstruction of high-density polyethylene into liquid hydrocarbon fuels and lubricants by hydrogenolysis over Ru catalyst

• DOI: 10.1016/j.checat.2021.04.002
• 发表时间: 2021-07-15
• 期刊: CHEM CATALYSIS
• 作者: Jia, Chuhua;Xie, Shaoqu;Lin, Hongfei
• 通讯作者: Lin, Hongfei

Assessing the Performance of Various Stochastic Optimization Methods on Chemical Kinetic Modeling of Combustion

• DOI: 10.1021/acs.iecr.0c04009
• 发表时间: 2020-10-28
• 期刊: INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
• 影响因子: 4.2
• 作者: Ashraf, Chowdhury;Pfaendtner, Jim
• 通讯作者: Pfaendtner, Jim