NSF-BSF: Deciphering Molecule-Carbon Nanotube Interactions for Environmental Remediation Reactions

NSF-BSF：破译环境修复反应中的分子-碳纳米管相互作用

• 批准号: 2129963
• 负责人: Hailiang Wang
• 金额: $ 54.69万
• 依托单位: Yale University
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2021
• 资助国家: 美国
• 起止时间: 2021-09-01 至 2024-08-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=2129963&HistoricalAwards=false
• 关键词: NSF; BSF; Deciphering; Molecule; Carbon

NSF-BSF: Deciphering Molecule-Carbon Nanotube Interactions for Environmental Remediation ReactionsElectrochemical reactions are emerging means to the efficient removal of environmentally concerning chemical species under mild reaction conditions, without the need for harsh chemical reactants, and powered by renewable energy sources. Nanostructured catalyst materials, especially those featuring multiple components with strong interactions, have greatly advanced the performance of many electrochemical reactions. However, the form and nature of these interactions and how they regulate the catalytic properties of the material remain elusive and is hampering both mechanistic understanding and performance optimization. In this project, in collaboration with researchers at the Hebrew University of Jerusalem, Dr. Hailiang Wang of Yale University and Dr. Robert Baker of the Ohio State University will combine materials synthesis, reaction studies, and spectroscopy techniques to perform detailed analysis of the nanoscale and molecular interactions between cobalt phthalocyanine, a metal coordination compound, and carbon nanotubes. Knowledge obtained from this research will be applied to reactions in carbon dioxide utilization and water purification. This project will also provide educational opportunities in environmental chemistry and engineering via outreach activities, classroom teaching, and research training to a diverse body of students in STEM fields. Dr. Hailiang Wang of Yale University and Dr. Robert Baker of the Ohio State University, in collaboration with researchers at the Hebrew University of Jerusalem, will analyze the nanoscale and molecular interactions between cobalt phthalocyanine and carbon nanotube and the ways by which these interactions can be utilized to optimize the electrocatalytic performance of the hybrid material for environmental applications. It is hypothesized those static interactions, i.e. electron relocation, controls the material’s thermodynamic behavior in the catalytic reaction, whereas dynamic interactions, i.e. the electron transfer rate, influences the catalytic kinetics. The team will leverage expertise in materials synthesis and reaction studies, high-spatial-resolution spectroscopy, and time-resolved spectroscopy to test the hypothesis. Static and dynamic interactions as functions of the material’s structural parameters, including the loading, dispersion, geometry, and linkage of cobalt phthalocyanine on carbon nanotube surface, will be analyzed. Fundamental structure-reactivity correlations will be established. Obtained mechanistic understanding will be utilized to further improve the environmental remediation reactions of carbon dioxide conversion to methanol and nitrate reduction by tailoring the nanoscale and molecular interactions. This project will also provide educational opportunities in environmental chemistry and engineering via outreach activities, classroom teaching, and research training to a diverse body of students in STEM fields.This research is jointly funded by NSF and The US-Israel Binational Science foundation through the special submission opportunity NSF 20-094.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.

NSF-BSF：用于环境修复反应反应反应的解密分子 - 碳纳米管相互作用是对在温和反应条件下的有效去除有关化学物种的环境的新兴手段，而无需HARMSH化学反应物，并且由可再生能源供电。纳米结构化催化剂材料，尤其是具有强烈相互作用的多个组件的材料，对许多电化学反应的性能进行了极大的提高。但是，这些相互作用的形式和性质及其如何调节材料的催化特性保持弹性，并且正在阻碍机械理解和性能优化。在该项目中，与希伯来大学希伯来大学的研究人员合作，耶鲁大学的Hailiang Wang博士和俄亥俄州立大学的Robert Baker博士将结合材料的合成，反应研究和光谱技术，以对纳米级和分子相互作用进行详细的分析，并将其分子相互作用。从这项研究中获得的知识将应用于二氧化碳利用和净水的反应。该项目还将通过外展活动，课堂教学以及为STEM领域的多元化学生体系提供宣传活动，课堂教学以及研究培训来为环境化学和工程提供教育机会。耶鲁大学的Hailiang Wang博士和俄亥俄州立大学的Robert Baker博士与耶路撒冷希伯来大学的研究人员合作，将分析钴苯甲酰氨基和碳纳米管之间的纳米级和分子相互作用，以及这些相互作用的方式可以通过效果进行效果，以使这些相互作用可用于造成电位效果。假设那些静态相互作用，即电子恢复，控制材料在催化反应中的热力学行为，而动态相互作用（即电子传递速率）影响催化动力学。该团队将利用材料合成和反应研究，高空间分辨率光谱和时间分辨光谱方面的专业知识来检验假设。将分析静态和动态相互作用作为材料结构参数的功能，包括碳纳米管表面上钴邻苯烷氨酸的负载，分散，几何和连锁。将建立基本的结构反应相关性。获得的机械理解将用于进一步改善二氧化碳转化为甲醇和硝酸盐还原的环境补救反应，并通过调整纳米级和分子相互作用。该项目还将通过宣传活动，课堂教学和研究培训在STEM领域的多样性团体中提供环境化学和工程学的教育机会。这项研究由NSF和美国 - 以色列双国科学基金会共同资助，通过专业提交机会NSF NSF 20-094，这些奖项通过评估NSF的智力及其在众多的启发下进行了评估。 标准。

项目成果

Aqueous Photoelectrochemical CO 2 Reduction to CO and Methanol over a Silicon Photocathode Functionalized with a Cobalt Phthalocyanine Molecular Catalyst

在钴酞菁分子催化剂功能化的硅光电阴极上将水相光电化学 CO 2 还原为 CO 和甲醇

• DOI: 10.1002/anie.202215213
• 发表时间: 2023
• 期刊: Angewandte Chemie International Edition
• 作者: Shang, Bo;Rooney, Conor L.;Gallagher, David J.;Wang, Bernie T.;Krayev, Andrey;Shema, Hadar;Leitner, Oliver;Harmon, Nia J.;Xiao, Langqiu;Sheehan, Colton
• 通讯作者: Sheehan, Colton