EFRI DCheM: Renewable Energy Driven Electrocatalytic Co-Conversion of CO2 and Regional Feedstocks to Chemicals and Fuels

该项目将通过迈向碳中和，节能和可分配的化学制造技术来应对实现可持续全球社会的重大挑战。PI将开发科学原理和技术，以制造分布式电化学反应器，同时修复CO2和升级搁浅的区域原料，以产生商品化学品和运输燃料。 具体地，电化学过程将使得能够使用可再生能源（例如，风能和太阳能）消耗来自固定源的CO2排放（例如，发电厂、化学精炼厂），但将以较低的能源需求来实现。该团队将通过使用单个反应器消耗二氧化碳并进行选择性氧化反应来实现这一目标，该反应器可以升级区域原料（例如，生物质、沼气）转化为有用的建筑砌块化学品。 PI将开发对界面化学的基本见解，以设计用于电化学氧化的新催化剂;应用反应工程原理来提高反应器的生产率和有效性;并分析关键资源的可用性和成本，以确定美国不同地区有前途的反应和反应器。 该团队将受益于高级人员，研究生和本科生中代表性不足的群体的人员，并将通过与电化学，制造，所提出的研究的变革性质在于将CO2的减少与共电解过程中区域原料的氧化升级联系起来。 这项工作利用了该团队最近的技术进步，即在碱性条件下将CO2高效流动电催化还原为乙烯和乙醇等C2产品，同时氧化废物，如生物燃料行业的甘油。具体而言，PI将通过合成和表征具有选择性氧化所需的多功能活性位点的新电催化剂，在流动的碱性条件下对阳极的表面化学和催化作用进行分子洞察。 该团队将设计，评估和优化液体电解质和膜基共电解反应器，用于耦合CO2还原和选择性氧化，重点是过程强化（例如，通过改变反应器-催化剂对的温度、压力、pH）。 该团队将使用技术经济分析和生命周期评估（TEA-LCA）与空间分辨资源数据来量化系统级水，能源和温室气体影响，以确定通过基于地理信息系统的多标准决策分析（GIS-MCDA）部署这些共电解设备的潜在机会。 研究重点之间的持续反馈将确保表面化学为反应器设计和工艺强化提供信息;性能指标更新TEA-LCA; TEA-LCA指导催化和反应器工程工作，以实现有希望的反应，并确定工艺的压力点。PI将提供多种共转化解决方案，每种方案都针对美国不同的地理区域进行了优化。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。

This project will address the grand challenge of achieving a sustainable global society by moving towards carbon-neutral, energy-efficient, and distributable chemical manufacturing technology. The PIs will develop the scientific principles and technology to make distributed electrochemical reactors that simultaneously remediate CO2 and upgrade stranded regional feedstocks in order to generate commodity chemicals and transportation fuels. Specifically, the electrochemical process will enable the use of renewable energy (e.g., wind and solar power) to consume CO2 emissions from stationary sources (e.g., power plants, chemical refineries) but will do so with lower energy requirements. The team will accomplish this by using a single reactor to consume CO2 and to perform selective oxidation reactions that upgrade regional feedstocks (e.g., biomass, biogas) into useful building block chemicals. The PIs will develop fundamental insight into interfacial chemistry to design new catalysts for electrochemical oxidations; apply reaction engineering principles to increase the productivity and effectiveness of the reactors; and analyze the availability and costs of critical resources to identify promising sets of reactions and reactors for distinct regions in the United States. The team will benefit from the inclusion of persons from underrepresented groups among senior personnel, graduate students, and undergraduate students and will engage local K-9 native Spanish speaker, Girl Scouts of Central Illinois, and other future members of the STEM workforce through unique educational programs related to electrochemistry, manufacturing, and sustainability.The transformative nature of the proposed research resides in linking the reduction of CO2 with the oxidative upgrading of regional feedstocks in a co-electrolysis process. This effort leverages the team's recent technological advances for energy-efficient flow electrocatalytic reduction of CO2 to C2-products such as ethylene and ethanol under alkaline conditions in tandem with oxidation of waste, such as glycerol from the biofuels industry. Specifically, the PIs will develop molecular insight into surface chemistry and catalysis at anodes in alkaline conditions under flow, by synthesizing and characterizing new electrocatalysts with multifunctional active sites needed for selective oxidations. The team will design, evaluate, and optimize liquid electrolyte and membrane-based co-electrolysis reactors for coupled CO2 reduction and selective oxidations with a focus on process intensification (e.g., by varying temperature, pressure, pH) for reactant-catalyst pairs. The team will use technoeconomic analysis and life cycle assessment (TEA-LCA) with spatially-resolved resource data to quantify system-level water, energy, and greenhouse gas impacts to identify potential opportunities to deploy these co-electrolysis devices via geographic information system based multicriteria decision analysis (GIS-MCDA). Constant feedback between the research thrusts will ensure that surface chemistry informs reactor design and process intensification; the performance metrics update the TEA-LCA; and TEA-LCA guides catalysis and reactor engineering efforts for promising reaction and identifies pressure points for the process. The PIs will deliver multiple co-conversion solutions, each optimized for a distinct geographical region in the US.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.