CAREER: Understanding Multiscale Mass Transport in Organic Electrosynthesis: Towards a Sustainable Pathway to Nylon Precursors

风能和太阳能可再生电力发电能力的增加为新的工业应用提供了减少环境足迹的机会。这个职业项目解决了用电而不是热化学方法制造普通化学中间体的关键问题。该项目将扩大对高性能电化学制造过程的设计和操作中的多尺度过程的基本理解。为了最好地实现这一目标，该项目将重点关注化学工业中最大的有机电化学反应作为模型反应：合成尼龙的前体己二腈（ADN）。 通过在多个长度尺度上探索运输和化学动力学现象，该项目将确定限制电化学反应器性能的关键因素，并推导出优化操作的设计规则。该项目将教育计划与培训可持续电化学行业未来劳动力的主要目标相结合。该教育计划包括来自西班牙裔背景的学生的K-12教育，电化学工程教育在本科和研究生化学工程课程中的整合，创业培训活动，和公众参与活动，以促进可持续的化学过程，通过时装业的影响。这个职业生涯项目提出了一个综合的研究和教育计划，其总体目标是了解多尺度在有机电合成中，穿过相关反应器区域的传输和动力学现象：近电极区域、本体液体电解质区域和离子传导膜。了解和控制发生在这三个区域的耦合过程可以提高转化率，选择性和能量转化效率，最终实现有机电合成反应器的工业大规模部署。为了更有效地实现项目目标，通过丙烯腈的电氢二聚电化学合成己二腈，将被用作模型反应。该项目分为三个研究重点。一号推力近电极工艺：推力1的目标是阐明的分子过程，通过研究他们与原位电化学光谱技术的选择性，然后使用这种理解来控制对所需的有机产品的选择性。2号推力 液体电解质工艺：推力2的目标是探索中尺度（10 -1000微米）多相电化学流动反应器中的传质和动力学过程之间的相互作用，然后使用所获得的知识来提高有机电合成反应器的性能。3号推力膜工艺：重点3的目标是了解有机电解质对离子传导膜的微观结构、渗透性和导电性的影响，并推导出膜分离有机电合成反应器的设计规则。该奖项反映了NSF的法定使命，并通过使用基金会的知识价值和更广泛的影响审查标准进行评估，被认为值得支持。

The increased generation capacity of renewable electricity from wind and solar offer new industrial applications with reduced environmental footprints. This CAREER project addresses key issues in the manufacture of common chemical intermediates using electricity rather than thermochemical means. The project will expand fundamental understanding of the multiscale processes in the design and operation of high-performing electrochemical manufacturing processes. To best achieve this goal, the project will focus on the largest organic electrochemical reaction implemented in the chemical industry as a model reaction: the synthesis of adiponitrile (ADN), a precursor to Nylon. By exploring transport and chemical kinetic phenomena at multiple length-scales, this project will identify key factors that limit the performance of electrochemical reactors and derive design rules for optimal operation. The project integrates an educational program with the primary objective of training a future workforce for a sustainable electrochemical industry. This educational program includes K-12 education of students from Hispanic background, integration of electrochemical engineering education in undergraduate and graduate chemical engineering curricula, entrepreneurship training activities, and public engagement activities to promote sustainable chemical processes through the influence of the fashion industry.This CAREER project presents an integrated research and education plan with the overarching goal of understanding multiscale transport and kinetic phenomena in organic electrosynthesis across the relevant reactor regions: the near-electrode region, the bulk liquid electrolyte region and ion conductive membranes. Understanding and controlling the coupled processes that take place at these three regions can result in improvements in conversion, selectivity, and energy conversion efficiency to ultimately enable the industrial large-scale deployment of organic electrosynthetic reactors. To more effectively accomplish the project goals, the electrochemical synthesis of adiponitrile via the electrohydrodimerization of acrylonitrile, will be used as a model reaction. The project is organized in three research thrusts. Thrust 1. Near-electrode processes: The goal of thrust 1 is to elucidate the molecular processes that drive selectivity by studying them with in situ electrochemical spectroscopy techniques and then use this understanding to control selectivity towards desired organic products. Thrust 2. Liquid electrolyte processes: The goal of thrust 2 is to explore the interplay between mass transport and kinetic processes in mesoscale (10's-1000's micrometers) multiphase electrochemical flow reactors and then use the knowledge gained to enhance performance of organic electrosynthesis reactors. Thrust 3. Membrane processes: The goal of thrust 3 is to understand the effects of organic electrolytes on the microstructure, permeability, and conductivity of ion-conducting membranes and to derive design rules for membrane-separated organic electrosynthesis reactors.This award reflects NSF's statutory mission and has been deemed worthy of support through evaluation using the Foundation's intellectual merit and broader impacts review criteria.