Reaction-Separation Processes for Production of Hydroxymethylfurfural from Fructose using Molecular Sieves

生物质作为化学品和燃料的碳中性来源的实际开发受到适合于亲水性、氧官能化和热不稳定的生物质原料的化学转化的工艺和反应工程技术的开发的限制。本研究旨在同时利用沸石材料的形状选择性催化性能和选择性分离，以在催化膜反应器中实施，这将使低温催化和分离过程能够转化糖单体，特别是将果糖脱水为羟甲基糠醛（HMF）。该项目基于初步数据，这些数据表明可以使用沸石膜选择性地从果糖中分离HMF，并寻求将PI先前的工作从用于烃分离的高选择性、高渗透性膜的合成扩展到集成反应分离系统和多功能生物质衍生原料。（沸石膜）、巴恩（沸石催化）和达乌什（过程设计和控制）研究小组，以开发使用生物质作为原料的新的反应-分离过程技术。具体而言，共同主要研究者计划：（i）使用稳态和化学/同位素瞬态实验研究确定果糖脱水的动力学、机理和位点要求，以提供用于工艺设计的反应速率的严格描述，（ii）研究沸石膜分离果糖衍生的氧官能化分子的潜力，并定量评估吸附和传输现象对HMF生产的速率和选择性的影响，和（iii）基于（i）和（ii）设计和优化集成反应-分离系统，并且，在工艺工程水平上比较和对比这种方法与其他反应吸附和反应-萃取两相系统的文献中提出的。研究包括相互作用的运输和吸附现象与动力学的反应系统的设计集成的低温反应-生物质原料的分离系统适用于生物质原料的特定分子结构，并将化学反应工程方法扩展到包括生物质加工在内的过程强化。更广泛的影响改变传统的化学加工和生产是全球社会面临的挑战之一，以确保可持续的未来。 催化剂开发、分离新材料和节能反应纯化工艺集成的结合有可能为这一转变做出贡献。 在这方面，这项研究将产生更广泛的方法影响，并可能刺激与生物炼制过程有关的其他问题的解决方案的发展。 共同PI将把这项工作的要素作为案例研究纳入高级本科生/研究生课程，重点是反应工程和分离，以及将在互联网上提供的教学模块。将鼓励本科生从事该项目的各个方面，并强调招聘工作，以确保合作PI研究小组内的持续多样性。

0855863TsapatsisThe practical exploitation of biomass as a carbon-neutral source of chemicals and fuels is limited by the development of process and reaction engineering technology suited for the chemical transformation of hydrophilic, oxygen-functionalized and thermally unstable biomass feedstock. This research seeks to simultaneously harness the shape selective catalytic properties of zeolitic materials and selective separations for implementation in catalytic membrane reactors that will enable low temperature catalytic and separation processes for conversion of sugar monomers, specifically for dehydration of fructose to hydroxymethylfurfural (HMF). It is predicated upon preliminary data that show HMF can be selectively separated from fructose using zeolite membranes and seeks to extend previous work from the PI on the synthesis of high-selectivity, high-permeability membranes for hydrocarbon separations to integrated reaction-separation systems and to polyfunctional biomass-derived feedstock.Intellectual Merit The project brings together the complementary and diverse experience of the Tsapatsis (zeolitic membranes), Bhan (zeolite catalysis) and Daoutidis (process design and control) research groups to develop new reaction-separation process technologies using biomass as feedstock. Specifically, the co-PIs plan to:(i) Determine the kinetics, mechanism and site requirements for the dehydration of fructose using steady state and chemical/isotopic transient experimental studies to provide a rigorous description of reaction rates for process design,(ii) Investigate the potential of zeolite-membranes to separate fructose-derived oxygenfunctionalized molecules and quantitatively assess the effect of adsorption and transport phenomena on the rate and selectivity of HMF production, and(iii) Design and optimize an integrated reaction-separation system based on (i) and (ii) and also, compare and contrast this methodology at a process engineering level with other reactionadsorption and reaction-extraction biphasic systems proposed in the literature.The research encompasses the interaction of transport and adsorption phenomena with kinetics in reaction systems for the design of integrated low-temperature reaction-separation systems adapted for the specific molecular structure of biomass feedstock and extends chemical reaction engineering approaches to process intensification to include biomass processing.Broader Impact Transforming traditional chemical processing and production is one of the challenges the global society faces to ensure a sustainable future. Combination of catalyst development, new materials for separations and energy efficient reaction-purification process integration has the potential to contribute to this transformation. In this respect, the research will have broader methodological impact and may stimulate the development of solutions for other problems related to biorefinery processes. The co-PIs will incorporate elements of this work as case studies in an advanced undergraduate/graduate course that focuses on reaction engineering and separations and in teaching-modules that will be made available on the internet. Undergraduate students will be encouraged to work on aspects of the project and emphasis will be given in recruiting efforts to assure continued diversity within the co-PIs research groups.