CAREER: Experimental Determination and Fundamental Theory of Mesoscopic Transport and Intrinsic Kinetics in CO2 Electrocatalysis

职业：二氧化碳电催化中介观输运和本征动力学的实验测定和基础理论

• 批准号: 2339693
• 负责人: Carlos Morales-Guio
• 金额: $ 68万
• 依托单位: University of California-Los Angeles
• 依托单位国家: 美国
• 项目类别: Continuing Grant
• 财政年份: 2024
• 资助国家: 美国
• 起止时间: 2024-03-01 至 2029-02-28
• 项目状态: 未结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=2339693&HistoricalAwards=false
• 关键词: CAREER; Experimental; Determination; Fundamental; Theory

The transformation of carbon dioxide (CO2) to fuels and chemicals using CO2 electrolyzers is a promising path forward for the electrification of the chemical manufacturing industry and the manufacturing of synthetic fuels for energy storage at a global scale. CO2 electrolyzers powered by electrons generated from wind and solar are key enabling technologies to achieve a zero-emissions future. Among the various metals studied for the electrochemical transformation of CO2, copper is the only single-element metal known to efficiently catalyze the production of multi-carbon oxygenates and hydrocarbons. There is still no consensus on how copper catalyzes this transformation. The rational design of future large-scale CO2 electrolyzers requires information on thermodynamics and reaction-transport kinetics. This project will address the research need of insufficient information on the reaction-transport kinetics on the copper catalyst system. This project will integrate results from research efforts into the training of undergraduate and graduate students at UCLA while also coordinating outreach activities to community colleges, minority serving institutions, national labs, and industries in California. The education and broadening impact activities include: i) development of a two year-summer research experience for chemical engineering undergraduate students. ii) outreach to industry and involvement of a diverse group of undergraduate and graduate students in research workshops and collaborations, and iii) introduction of electrochemical engineering concepts, cells, and theories developed in this proposal in the undergraduate chemical engineering capstone course, and the electrochemical processes course taught by the PI. Recently, it has become evident that transport is on equal footing with intrinsic catalytic kinetics of copper active sites in determining reaction mechanisms and product distributions of CO2 electroreductions, and thus a detailed extraction of reaction kinetics under well-defined mass, heat and charge transport conditions is necessary. This fundamental engineering research project addresses the critical need for the determination and modeling of mesoscopic transport and reaction kinetics relevant to CO2 electrocatalysis by combining: i) reactor design and characterization, ii) accelerated collection, ingestion, and contextualization of large experimental datasets to enable the decoupling of transport contributions from CO2 reduction kinetics, and iii) the development and parametrization of multi-scale reaction-transport models. The reaction-transport model developed here will be the first of its kind for electrochemical CO2 reduction and should enable the future rational design and scale-up of CO2 electrolyzers. The research will explore how mass, heat and charge transport determine product selectivity in CO2 reduction and will develop the fundamental theory and tools needed to build a reaction-transport model of electrocatalytic processes on copper electrodes. Electrochemical cells with well-defined transport properties will be utilized as tools to generate large experimental datasets of correlations between six experimental variables (applied potential, transport characteristics in the cell, electrolyte composition, temperature, pressure and catalyst porosity) and the production rates for 16 different liquid and gas products on copper catalysts. This large dataset will be of high quality and will be used to determine the underlying CO2 reduction mechanism on copper electrodes and the contribution of external and internal mass, heat and charge transport effects on the generation of different product distributions observed on catalysts with different porosities.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.

二氧化碳（CO2）使用二氧化碳和化学物质的转化是化学制造业电气化和制造合成燃料以在全球范围内存储的合成燃料的有前途的途径。由风和太阳能产生的电子提供动力的二氧化碳电解器是实现未来零排放的关键技术。在研究CO2电化学转化的各种金属中，铜是已知有效催化多碳氧合和碳氢化合物的产生的唯一单元金属。关于铜如何催化这种转化，仍然没有共识。未来大规模二氧化碳电解器的合理设计需要有关热力学和反应传输动力学的信息。该项目将解决有关铜催化剂系统中反应传输动力学的信息的研究需求。该项目将将研究工作的结果纳入加州大学洛杉矶分校的本科生和研究生的培训，同时还向加利福尼亚州的社区学院，少数派服务机构，国家实验室和行业协调外展活动。教育和扩大影响活动包括：i）为化学工程本科生提供两年夏季研究经验。 ii）对工业的宣传以及一组不同的本科生和研究生参与研究研讨会和协作的参与，以及iii）在本科化学工程工程帽集结课程以及PI由PI教授的电化学过程的本科化学工程工程课程中，引入了电化学工程概念，细胞和理论。最近，已经很明显的是，在确定二氧化碳电源的反应机理和产物分布中，运输与铜活性位点的固有催化动力学处于同等的基础上，因此必须在明确定义的质量，热量和电荷传输条件下详细提取反应动力学。这个基本的工程研究项目解决了确定和建模与CO2电催化相关的介质运输和反应动力学的关键需求：反应传输模型。此处开发的反应传输模型将是减少电化学二氧化碳的第一个此类模型，并应实现二氧化碳电解器的未来理性设计和扩展。该研究将探讨质量，热和电荷传输如何确定二氧化碳中的产品选择性，并将开发铜电极上电催化过程的反应传输模型所需的基本理论和工具。具有明确定义的运输特性的电化学细胞将被用作产生六个实验变量之间相关性的大型实验数据集（应用电位，电池中的传输特性，电解质组成，温度，压力和催化剂孔隙率）和铜催化剂上16种不同的液体和天然气产物的生产速率。这个大型数据集将具有高质量的质量，并将用于确定铜电极上的基本二氧化碳减少机制以及外部和内部质量，内部和内部质量，热量和电荷运输对在具有不同孔隙率的催化剂上观察到的不同产品分布的影响的贡献。该奖项反映了NSF的法定任务，并反映了通过评估范围的Intellitia和Forligia的支持者，并反映了基础的支持者，并反映了基础的支持。