Collaborative Research: Electrochemical Reduction of CO2 to Small Organic Fuels on Encapsulated Metal Catalysts in Gas Diffusion Electrode Environment

合作研究：气体扩散电极环境中封装金属催化剂将二氧化碳电化学还原为小分子有机燃料

• 批准号: 1235654
• 负责人: Christopher Williams
• 金额: $ 12万
• 依托单位: University of South Carolina at Columbia
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2012
• 资助国家: 美国
• 起止时间: 2012-09-01 至 2015-08-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1235654&HistoricalAwards=false
• 关键词: Collaborative; Research; Electrochemical; Reduction; CO2

PI: Li, Wenzhen / Williams, ChristopherProposal Number: 1235982 / 1235654Institution: Michigan Technological University / University of South Carolina at ColumbiaTitle: Collaborative Research: Electrochemical Reduction of CO2 to Small Organic Fuels on Encapsulated Metal Catalysts in Gas Diffusion Electrode EnvironmentThe increase of the greenhouse gas CO2 in the atmosphere has resulted in serious global warming issues. The electroreduction of CO2 to organic molecules is a critical goal that would positively impact the global carbon balance by recycling CO2 back into usable fuels. However, an electroreduction that is fast enough and can operate to full capacity remains a great scientific challenge. This collaborative team proposes to investigate a novel class of carbon nanotube (CNT) encapsulated Cu-based nanostructures for efficient electrocatalytic reduction of CO2 in gas diffusion phase, based on their extensive research expertise in catalysis, spectroscopy and electrochemical engineering. The research hypotheses are: 1) that inside CNT channels, CO2 and H species transport and charge transfer can be effectively tuned through optimizing the diameter and length of CNTs and distribution of metal nanoparticles; 2) that the spatial restriction of CNT channels can enhance chain growth probability (to form C2+ fuels); 3) that the cation exchange ionomer can effectively adjust the local pH of reaction sites close to neutral in order to facilitate CO2 reduction. The project will focus on three research tasks: 1) rationally design, accurately synthesize and fully characterize CNTs encapsulated Cu- based bimetallic (Fe, Ag, Pd, etc) nanoparticles having alloy or core-shell structure; 2) investigate mechanistic steps of CO2 reduction at the encapsulated catalyst-cation exchange membrane ionomer interface using in-situ electrochemical FTIR, gas chromatography-mass spectrometry and high performance liquid chromatography; 3) assemble encapsulated catalysts into MEAs and investigate CO2 reduction in gas diffusion electrode environment using electrochemical methods, chromatography analysis, and micro-kinetic modeling.This research will have several broad scientific and social impacts. First, studies of these novel encapsulated catalytic systems will advance knowledge of precise synthesis of composite catalytic materials and structure-catalytic function relationships. Second, the research efforts will deepen our understanding of electro-driven conversion of CO2 to usable organic fuels (electrofuels). Third, it will advance CO2 conversion knowledge based on solid polymer electrolyte and gas diffusion electrode techniques and support the world-wide research efforts to balance global carbon cycling and alleviate global climate change issues. The students involved will not only acquire hands-on research skills, but also learn analytical, communication, cooperation and innovation skills. In addition, the PIs will incorporate the generated results into the existing undergraduate courses and enterprise projects. The outreach efforts will increase high school students? interests in science, engineering and technology, and eventually benefit our society by a sustainably supply of new generation researchers in these fields.

主要研究者：Li，Wenzhen /威廉姆斯，Christopher提案编号：1235982 /1235654机构：密歇根理工大学/南卡罗来纳州大学哥伦比亚分校题目：合作研究：在气体扩散电极环境中在封装金属催化剂上电化学还原CO2为小有机燃料大气中温室气体CO2的增加导致了严重的全球变暖问题。将CO2电还原为有机分子是一个关键目标，它将通过将CO2回收为可用燃料来积极影响全球碳平衡。然而，足够快并且可以满负荷运行的电还原仍然是一个巨大的科学挑战。该合作团队建议研究一类新型的碳纳米管（CNT）封装的铜基纳米结构，用于在气体扩散阶段有效地电催化还原CO2，基于他们在催化，光谱学和电化学工程方面的广泛研究专业知识。研究假设是：1）通过优化碳纳米管的直径和长度以及金属纳米颗粒的分布，可以有效地调节碳纳米管通道内CO2和H物种的输运和电荷转移; 2）碳纳米管通道的空间限制可以提高链增长概率（形成C2+燃料）; 3）阳离子交换离聚物能有效地调节反应位点的局部pH值，使其接近中性，有利于CO2的还原。本项目将围绕三个方面开展研究工作：1）合理设计、准确合成和全面表征碳纳米管包覆铜基复合材料具有合金或核-壳结构的（Fe、Ag、Pd等）纳米颗粒; 2）利用原位电化学FTIR研究了CO2在包封催化剂-阳离子交换膜离聚物界面上还原的机理步骤，气相色谱-质谱联用仪和高效液相色谱仪; 3）将封装催化剂组装到MEA中，并利用电化学方法、色谱分析和微观动力学模型研究气体扩散电极环境中CO2的还原。首先，这些新型封装催化体系的研究将推进复合催化材料的精确合成和结构-催化功能关系的知识。第二，研究工作将加深我们对CO2到可用有机燃料（电燃料）的电驱动转化的理解。第三，它将推进基于固体聚合物电解质和气体扩散电极技术的CO2转化知识，并支持全球范围内平衡全球碳循环和缓解全球气候变化问题的研究工作。 参与的学生不仅将获得实践研究技能，还将学习分析，沟通，合作和创新技能。此外，PI将把产生的结果纳入现有的本科课程和企业项目。外展工作将增加高中生？我们的目标是培养对科学、工程和技术感兴趣的人，并最终通过可持续地提供这些领域的新一代研究人员来造福我们的社会。