Interplay of Mass Transport and Chemical Kinetics in the Electroreduction CO2

电还原 CO2 中传质与化学动力学的相互作用

• 批准号: 1803482
• 负责人: Chao Wang
• 金额: $ 30万
• 依托单位: Johns Hopkins University
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2018
• 资助国家: 美国
• 起止时间: 2018-09-01 至 2021-08-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1803482&HistoricalAwards=false
• 关键词: Interplay; Mass; Transport; Chemical; Kinetics

Electrochemical reduction of carbon dioxide (CO2), a way of carbon recycling or carbon reuse, represents a promising solution for energy and environmental sustainability. Despite the great potential for storage of renewable energy and sustainable production of hydrocarbon chemicals and fuels, the electroreduction of CO2 is challenged by the lack of efficient electrocatalysts. Both the surface structure of the catalysts and mass transport through the nanostructured electrodes play important roles in CO2 reduction to higher order carbon products. This research will develop fundamental understanding of the interplay between mass transport and chemical kinetics in the electroreduction of CO2 by integrating experimental and simulation studies. The project will also foster the growth of the next generation of engineers to address global challenges in energy and environmental sustainability. This will be achieved by training graduate students with state-of-the-art experimental and theoretical skills and developing their independent research philosophy, providing undergraduate and high-school students with hands-on experiences at the cutting-edge of science and engineering research, and educating and mentoring K-12 students from diverse backgrounds to consider careers in STEM fields.This fundamental engineering science project will advance the mechanistic understanding of the mass transport and chemical kinetics in CO2 electrolysis. This project integrates experimental and computational studies through the following efforts: i) synthesis and characterization of a model high surface area catalyst consisting of highly dense copper (Cu) nanowires grown on 2D Cu mesh; ii) systematic electrocatalytic studies using Cu nanowires prepared under different reaction conditions and with distinct nanoscale and surface structures; iii) characterization studies of the surface structures and properties of the Cu nanowires to understand the structure effect on the chemical kinetics; and iv) transport modeling that takes into account the diffusion, migration and reaction consumption of chemical species through the Cu nanowires to understand the mass transfer effects on the electrocatalytic performance of high-surface-area electrodes. The expected outcomes of this project will reduce the knowledge gap by correlating the nanostructures of Cu electrocatalysts to their catalytic performances. The mass transport modelling effort emphasizes the importance of understanding both spatial architecture-dependent mass transport and surface-structure dependent chemical kinetics. The fundamental understanding to be developed in this research serves as guidelines for the further development of advanced electrocatalysts toward improved energy efficiency, power performance and product selectivity of CO2 electrolyzers.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.

二氧化碳的电化学还原是碳循环或碳再利用的一种方式，是能源和环境可持续发展的一种很有前途的解决方案。尽管可再生能源的储存和碳氢化合物化学品和燃料的可持续生产具有巨大潜力，但由于缺乏有效的电催化剂，二氧化碳的电还原面临着挑战。催化剂的表面结构和通过纳米结构电极的传质都对二氧化碳还原为高阶碳产品起着重要作用。这项研究将通过实验和模拟研究相结合的方式，加深对二氧化碳电还原过程中质量传输和化学动力学之间相互作用的基本理解。该项目还将促进下一代工程师的成长，以应对能源和环境可持续性方面的全球挑战。这将通过以下方式实现：培训研究生掌握最先进的实验和理论技能，发展他们的独立研究哲学，为本科生和高中生提供科学和工程研究前沿的实践经验，以及教育和指导来自不同背景的K-12学生考虑在STEM领域就业。这个基础工程科学项目将促进对二氧化碳电解中质量传输和化学动力学的力学理解。本项目通过以下工作将实验和计算研究融为一体：i)合成和表征由在2D Cu网上生长的高密度铜(Cu)纳米线组成的模型高比表面积催化剂；ii)使用在不同反应条件下制备的具有不同纳米和表面结构的铜纳米线进行系统的电催化研究；iii)对铜纳米线的表面结构和性质进行表征研究，以了解结构对化学动力学的影响；以及iv)传输模拟，考虑化学物种通过铜纳米线的扩散、迁移和反应消耗，以了解传质对高表面积电极电催化性能的影响。该项目的预期结果将通过将铜电催化剂的纳米结构与其催化性能相关联来缩小知识差距。质量传输模型工作强调了理解依赖于空间结构的质量传输和依赖于表面结构的化学动力学的重要性。这项研究将形成的基本理解将作为进一步开发先进电催化剂的指导方针，以提高二氧化碳电解槽的能效、动力性能和产品选择性。该奖项反映了NSF的法定使命，并通过使用基金会的智力优势和更广泛的影响审查标准进行评估，被认为值得支持。

项目成果

Nano-folded Gold Catalysts for Electroreduction of Carbon Dioxide

• DOI: 10.1021/acs.nanolett.9b04564
• 发表时间: 2019-12-01
• 期刊: NANO LETTERS
• 影响因子: 10.8
• 作者: Kwok, Kam Sang;Wang, Yuxuan;Gracias, David H.
• 通讯作者: Gracias, David H.