EAGER: Mechanistic and Stability Studies over Dual-Function Materials for CO2 Capture and Conversion

该项目研究温室气体二氧化碳(CO2)与氢气(H2)的化学反应，以生产甲醇，用于发电(通过甲醇燃料电池)或用作合成各种燃料和化学产品的平台化学品。与这一早期概念探索性研究奖助金(AGER)项目相关的新功能包括：1)探索一种反应工程方法，涉及由双反应堆实现的循环二氧化碳捕获-转化；2)整合新的实验能力，使研究能够在商业反应堆的高压下进行。更广泛地说，该项目研究了一种战略，通过就地捕获产生的二氧化碳并将其与氢气(从使用可持续能源的水中获得)转化为甲醇来结束碳循环。这个急切的项目是从调查员的职业项目衍生出来的。CARAPE项目专注于双功能材料(DFM)的合成和评估，该材料能够捕获和转化二氧化碳，并相应地避免了与二氧化碳捕获和封存相关的能源需求、腐蚀和运输问题。该项目满足了迫切的标准，因为在将废物二氧化碳转化为甲醇和其他高价值分子的过程中，对转化潜力与与动力学和热力学挑战相关的固有风险进行了权衡。因此，该项目为化学品和燃料的低温室气体生产或净零温室气体生产提供了一个循环的切入点。例如，在燃料的情况下，甲醇(或衍生燃料产品)的燃烧将产生二氧化碳，可通过启动反应循环回甲醇。该项目将开发进行二氧化碳捕获-转化循环研究的方法，使二氧化碳捕获发生在第一个反应堆中，而转化发生在第二个反应堆中，每隔几分钟切换一次。从能量的角度来看，该系统在等温等压条件下运行是有益的。该项目由一名经验丰富的博士后助理带来的技术专长加强，他将在PI的指导下发展成功的独立研究生涯所需的领导力和项目管理技能。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。

The project investigates the chemical reaction of carbon dioxide (CO2), a greenhouse gas, with hydrogen (H2) to produce methanol for either energy generation (via methanol fuel cells) or use as a platform chemical for the synthesis of a wide range of fuel and chemical products. Novel features associated with this Early-concept Grant for Exploratory Research (EAGER) project include 1) exploring a reaction engineering approach involving cyclic CO2 capture-conversion enabled by dual reactors and 2) incorporating new experimental capabilities allowing research at high pressures characteristic of commercial reactors. More broadly, the project investigates a strategy to close the carbon cycle by in-situ capture of produced CO2 and its conversion with H2 (obtained from water using sustainable energy) to methanol. The EAGER project is a spinoff from the investigator's CAREER project. The CAREER project is focused on the synthesis and evaluation of dual-function materials (DFMs) capable of both capturing and converting CO2, with corresponding benefits of avoiding energy demands, corrosion, and transportation issues associated with CO2 capture and sequestration. The project fulfills the EAGER criteria in that the transformative potential is weighed against the inherent risk associated with kinetic and thermodynamic challenges in converting waste CO2 to methanol and other high-value molecules. The project thus provides an entry point to circularity in low- or net-zero greenhouse gas production of chemicals and fuels. For example, in the fuel case, the combustion of methanol (or derivative fuel products) will generate CO2 that can be cycled back to methanol via the starting reaction. The project will develop methods to conduct CO2 capture-conversion cyclic studies in such a way that the CO2 capture takes place in the first reactor while the conversion occurs in the second one, with switching every few minutes. From an energetic point of view, the system benefits from operation under isothermal and isobaric conditions. The project is enhanced by technical expertise brought by an experienced post-doctoral associate, who will be mentored by the PI in developing leadership and project management skills needed for a successful independent research career.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.