CAREER: Electrochemically Mediated Carbon Dioxide Separation via Non-Aqueous Proton-Coupled Electron Transfer

职业：通过非水质子耦合电子转移进行电化学介导的二氧化碳分离

• 批准号: 2237096
• 负责人: Yayuan Liu
• 金额: $ 51.57万
• 依托单位: Johns Hopkins University
• 依托单位国家: 美国
• 项目类别: Continuing Grant
• 财政年份: 2023
• 资助国家: 美国
• 起止时间: 2023-07-01 至 2028-06-30
• 项目状态: 未结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=2237096&HistoricalAwards=false
• 关键词: CAREER; Electrochemically; Mediated; Carbon; Dioxide

The efficient capture of carbon dioxide (CO2) from stationary emitters and ambient air is vital in meeting climate targets. However, the conventional thermochemical methods for CO2 capture are energy-intensive, cost-prohibitive, and fossil fuel-dependent. On the other hand, emerging carbon capture approaches driven by electrochemical reactions promise mild operating conditions, flexibility for coupling to intermittent renewable energy resources, and could accommodate the multi-scale nature of carbon capture needs due to their modularity. Nevertheless, the practical deployment of existing electrochemical carbon capture processes remains hindered by issues such as oxygen sensitivity and evaporative loss. Correspondingly, this project explores a new concept for carbon capture modulated by electrochemical stimuli. The concept involves the generation of low-volatility, air-stable CO2 sorbents at an electrode surface, followed by CO2 capture in an absorber unit and the subsequent CO2 release upon switching the polarity of the electrode. The goal is to understand and ultimately harness control over the thermodynamics, reaction kinetics, and transport properties of the model electrochemical system, utilizing a multi-modal toolkit of materials synthesis, characterization, and electroanalysis. The broader impacts involve education and mentoring activities from high school through graduate levels to prepare a young generation of engineers with an interdisciplinary skillset essential to solving humanity’s sustainability challenges, which include developing high school laboratory modules on carbon capture and integrating advances in separation methods and interfacial sciences into the university’s chemical engineering curriculum. The project aims to research an electrochemical interface composed of redox-tunable Brønsted base moieties that can undergo proton-coupled electron transfer (PCET) in non-aqueous electrolytes for the reversible (re)generation of air-stable CO2 sorbents. At the molecular level, the relationship between molecular structure, Brønsted basicity, and PCET energetics will be delineated to inform the rational design of carbon capture chemistry. At the material level, microporous electrodes will be synthesized to examine the interplay between electrode microstructure and the corresponding mass and charge transport behaviors. The impact of the electrolyte environment on the PCET and CO2 chemisorption kinetics will also be systematically investigated via (electro)analytical techniques. Finally, the CO2 separation concept will be evaluated in a bench-scale prototype, and a combined experimental and modeling effort will shed light on possible degradation mechanisms and bottlenecks to promote rationally motivated improvement strategies.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.

从固定发射器和环境空气中有效捕获二氧化碳（CO2）对于满足气候目标至关重要。但是，用于二氧化碳捕获的常规热化学方法是能源密集型，成本良好的和化石燃料依赖性的。另一方面，新兴的碳捕获方法通过电化学反应推动了轻度的操作条件，耦合的灵活性与可再生能源可再生能源，并且可以满足碳捕获需求的多尺度性质。然而，现有的电化学碳捕获过程的实际部署仍然受到氧气灵敏度和蒸发损失等问题的阻碍。相应地，该项目探讨了通过电化学刺激调制的碳捕获的新概念。该概念涉及在电极表面生成低挥发性，空气稳定的二氧化碳吸附剂，然后在吸收器单元中捕获二氧化碳，然后在切换电极的极性后随后的二氧化碳释放。目的是利用材料合成，表征和电分析的多模式工具包，了解模型电化学系统的热力学，反应动力学和传输特性，并最终利用并最终利用控制模型电化学系统的控制。更广泛的影响涉及从高中到研究生水平的教育和心理活动，以使年轻一代工程师为解决人类的可持续发展挑战至关重要，其中包括在分离方法中开发高中实验室模块，并将其整合到分离方法中，并将其整合到大学的化学工程学课程中。该项目旨在研究由氧化还原可调的Brønsted碱基部分组成的电化学界面，该界面可以在非水晶的非液体电解质中进行质子耦合的电子传输（PCET），以用于可逆（RE）生成气稳定的CO2香水。在分子水平上，将划定分子结构，Brønsted碱性和PCET Energys之间的关系，以告知碳捕获化学的合理设计。在材料水平上，将合成微孔电子，以检查电子微结构与相应质量和电荷传输行为之间的相互作用。电解质环境对PCET和CO2化学吸附动力学的影响也将通过（电）分析技术系统地研究。 Finally, the CO2 separation concept will be evaluated in a bench-scale prototype, and a combined experimental and modeling effort will shed light on possible degradation mechanisms and bottlenecks to promote rationally motivated improvement strategies.This award reflects NSF's statutory mission and has been deemed precious of support through evaluation using the Foundation's Intellectual merit and broader impacts review criteria.