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

0855863 tsapatsis生物质作为一种碳中性的化学品和燃料来源的实际开发受到适合于亲水性、氧功能化和热不稳定生物质原料化学转化的过程和反应工程技术的发展的限制。本研究旨在同时利用沸石材料的形状选择性催化特性和选择性分离，在催化膜反应器中实现糖单体转化的低温催化和分离过程，特别是果糖脱水到羟甲基糠醛（HMF）。该研究基于初步数据，表明HMF可以使用沸石膜选择性地从果糖中分离出来，并试图将PI之前关于合成高选择性、高渗透性碳氢化合物分离膜的工作扩展到综合反应分离系统和多功能生物质衍生原料。该项目汇集了Tsapatsis（沸石膜）、Bhan（沸石催化）和Daoutidis（过程设计和控制）研究小组的互补性和多样化经验，以开发使用生物质作为原料的新型反应分离过程技术。具体来说，co- pi计划：(i)确定动力学；利用稳态和化学/同位素瞬态实验研究，为工艺设计提供反应速率的严格描述；（ii）研究沸石膜分离果糖衍生的氧功能化分子的潜力，定量评估吸附和运输现象对羟甲基糠醛生产速率和选择性的影响；（iii）基于(i)和（ii）设计和优化一个集成的反应分离系统，同时，在工艺工程水平上将该方法与文献中提出的其他反应吸附和反应萃取双相系统进行比较和对比。该研究涵盖了反应系统中运输和吸附现象与动力学的相互作用，用于设计适合生物质原料特定分子结构的综合低温反应分离系统，并将化学反应工程方法扩展到过程强化，包括生物质处理。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-净化过程整合的结合有可能促进这一转变。在这方面，这项研究将在方法上产生更广泛的影响，并可能促进发展与生物炼制过程有关的其他问题的解决办法。合作pi将把这项工作的元素作为案例研究纳入高级本科/研究生课程，该课程侧重于反应工程和分离，并将在互联网上提供教学模块。本科学生将被鼓励在项目的各个方面工作，并将重点放在招聘工作上，以确保共同pi研究小组的持续多样性。

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.