SusChEM: Directing the distribution of biomass-derived molecules in porous materials

项目负责人姓名：Susannah L. scott提案号：1512228通过使用非粮食生物质等可再生资源，可以实现重要化学品和燃料的大规模可持续生产。利用多孔固体催化剂将生物质衍生的碳水化合物在液态水中选择性地转化为特定的化学物质，部分是由生物质衍生的碳水化合物分子运动到催化剂的多孔结构中，以及产物从多孔结构中运动出来控制的。该项目将研究水、催化剂孔结构、碳水化合物和产品之间相互作用的基础科学，使用高分辨率测量技术探测这些材料的分子相互作用。研究结果可能为调整催化过程提供建议，以在更短的时间内获得更高的收率和产物的选择性。通过这项研究，学生将有机会在太平洋西北国家实验室的环境分子科学实验室接受高级培训。本研究的总体目标是了解多孔催化剂中水、生物质衍生碳水化合物和呋喃基产品之间的相互作用。在大量生产碳基燃料和化学品所需的规模上，木质纤维素生物质的使用可能涉及在许多化学转化步骤中使用多相催化剂的连续液相处理。反应介质的各种组分，包括溶剂、反应物、中间体和产物，将在多孔催化剂材料内划分。根据对有机溶剂与水结合的混合溶剂系统中显著效应的观察，假设分子对孔隙的不同吸收及其在孔壁上的特定吸附对选择性有深远的影响。为了在分子水平上阐明界面约束的本质并量化这些相互作用的程度，该研究将使用非原位和原位固态核磁共振（NMR）监测固液界面，通过使用特别设计的高温高压魔角旋转探针，评估碳水化合物衍生分子的局部结构及其在沸石等多孔材料中的转化速率。介孔硅和有机硅，还有碳。这些信息将与探测吸收/吸附现象热力学的量热测量和探测其动力学的重量测量相结合。作为这项研究的一部分，学生将通过太平洋西北国家实验室的环境分子科学实验室接受先进核磁共振技术的培训。对界面受限物质行为的了解将有助于确定选择反应物、促进所需反应和排出特定所需产物（如呋喃）的孔隙结构。

PI Name: Susannah L. ScottProposal Number: 1512228The sustainable production of important chemicals and fuels at large scale can be achieved by using renewable resources such as non-food biomass. The selective conversion of biomass-derived carbohydrates to specific chemicals in liquid water using porous solid catalysts is controlled in part by the molecular movement of biomass derived carbohydrate molecules into the porous structure of the catalyst, as well as the movement of products out of the porous structure. This project will study the fundamental science underlying the interactions between water, catalyst pore structure, carbohydrates, and products using high resolution measurement techniques which probe the molecular interactions of these materials. The outcomes of the research may suggest ways to adjust the catalysis process to achieve higher yield and selectivity of products in shorter times. Through this research, students will be given opportunities for advanced training at the Environmental Molecular Sciences Laboratory at Pacific Northwest National Laboratory.The overall goal of this research is to understand the interactions between water, biomass-derived carbohydrates, and furan-based products within porous catalysts. The use of lignocellulosic biomass on the scale required for significant production of carbon-based fuels and chemicals will likely involve continuous liquid-phase processing with heterogeneous catalysts in many of the chemical conversion steps. Various components of the reaction medium, including solvent, reactants, intermediates and products, will partition within the porous catalyst material. Differential absorption of molecules into the pores and their specific adsorption onto the pore walls are hypothesized to have profound consequences for selectivity, based on observations of dramatic effects in mixed solvent systems where an organic solvent is combined with water. To elucidate the nature of the interface confinement at the molecular level and to quantify the extent of these interactions, the research will use ex-situ and in-situ solid-state nuclear magnetic resonance (NMR) monitoring of solid-liquid interfaces, via the use of specially designed high temperature-high pressure magic-angle-spinning probes, to assess local structures of carbohydrate-derived molecules and their rates of transformations in porous materials such as zeolites, mesoporous silicas and organosilicas, and carbons. This information will be combined with calorimetric measurements that probe the thermodynamics of absorption/adsorption phenomena, and gravimetric measurements to probe their kinetics. As part of this research, students will be trained on advanced NMR techniques through the Environmental Molecular Sciences Laboratory at Pacific Northwest National Laboratory. Knowledge gained on the behavior of interface-confined species will identify pore structures that select for reactants, promote desired reactions and expel specific desired products, such as furanics.