Collaborative Research: SUSCHEM: Engineering Polymer-Nanocatalyst Membranes for Direct Capture of CO2 and Electrochemical Conversion to C2+ Liquid Fuel

合作研究：SUSCHEM：用于直接捕获 CO2 和电化学转化为 C2 液体燃料的工程聚合物纳米催化剂膜

• 批准号: 2324345
• 负责人: Shouheng Sun
• 金额: $ 30万
• 依托单位: Brown University
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2023
• 资助国家: 美国
• 起止时间: 2023-10-01 至 2026-09-30
• 项目状态: 未结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=2324345&HistoricalAwards=false
• 关键词: Collaborative; Research; SUSCHEM; Engineering; Polymer; Collaborative; Research; SUSCHEM; Engineering; Polymer

There have been rising environmental concerns resulting from the increasing emission of greenhouse gasses like CO2. One effective way to manage CO2 level is to directly capture and convert CO2 from air to other carbon forms. The direct conversion of CO2 using air as feedstock to a reusable carbon product has been extremely difficult and current approaches often involve an additional energy-intensive step to produce pure CO2 as feedstock for subsequent catalytic conversion. This proposal will address the current unmet challenges to allow direct air capture with a minimum energy input on capture/release and sequential electroreduction of CO2 to value-added liquid fuels. The concept is based on the design of a novel bioinspired process. The central component is a cellulose-based membrane that is used directly for capture and separation of CO2 from air. This new capture reaction, not yet been studied previously, will provide a very powerful processing tool for direct air capture of CO2. To convert CO2 to a reusable form of carbon, a new class of earth-abundant cobalt catalyst (hexagonal close packed cobalt nanosheets) will be studied. The capture and conversion will be realized conveniently via the cellulose-graphene-cobalt system in which local basicity and CO2 proximity to the catalyst are rationally controlled to facilitate efficient electroreduction of CO2. Through collaborative efforts between Brown and UConn, the proposed studies will generate an innovative design of an all-in-one integrated system to realize sustainable CO2 capture and utilization.This proposal aims to develop a novel electrochemical system for direct air capture and conversion of CO2 to ethanal and/or ethanol under ambient conditions. The system consists of natural cellulose and a new hexagonal cobalt nanosheet catalyst deposited on graphene, providing a highly conductive and porous polymer network where the two components work cooperatively in direct air capture and electroreduction of CO2. Hydroxyl-rich amorphous cellulose can capture CO2 in the form of metastable hemi-carbonates catalyzed by a base. These metastable hemi-carbonates can reversibly release CO2 upon pH change or gentle heating, providing an energy-efficient approach to CO2 capture and release, which is inspired by natural CO2 concentration mechanisms in photosynthesis. The released CO2 is in proximity of the robust cobalt nanosheet catalyst assembled on graphene and integrated into the cellulose membrane, which functions as a working electrode to carry out the selective electroreduction of CO2 to C2 products. A working flow-cell system will be demonstrated as an engineering approach to direct capture and conversion of CO2 with air as feedstock. The study will offer not only a new design concept on cellulose processing method and new fundamental knowledge on the cobalt nanosheet-promoted C-C coupling in the CO2 reduction reaction, but also an energy-efficient engineering solution to direct CO2 capture and conversion.The portion of this project that will be completed at Brown University is jointly funded by the Electrochemical Systems Program and the Established Program to Stimulate Competitive Research (EPSCoR).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.

由于二氧化碳等温室气体的排放越来越高，环境问题引起了人们的关注。管理二氧化碳水平的一种有效方法是将二氧化碳从空气直接捕获并将其转换为其他碳形式。使用空气作为原料与可重复使用的碳产品的直接转化非常困难，目前的方法通常涉及一个额外的能源密集型步骤，以生产纯二氧化碳作为原料，以进行随后的催化转化。该提案将解决当前未满足的挑战，以允许在捕获/释放和将CO2的顺序释放到增值的液体燃料的捕获/释放和连续的电量时进行直接捕获。该概念基于新型生物启发过程的设计。中心成分是一种基于纤维素的膜，直接用于捕获和与空气中的二氧化碳分离。以前尚未研究这种新的捕获反应将为直接空气捕获CO2提供非常强大的处理工具。为了将二氧化碳转换为可重复使用的碳，将研究一种新的土壤丰富的钴催化剂（六角形近距离堆积的钴纳米片）。捕获和转化将通过纤维素 - 含碳酸盐铜系统方便地实现，在该系统中，局部碱性和与催化剂的近端合理控制以促进二氧化碳的有效电化。通过Brown和UConn之间的合作努力，拟议的研究将对一个多合一的集成系统进行创新设计，以实现可持续的CO2捕获和利用。该提案旨在在环境条件下直接捕获CO2和/或乙醇的新型电化学系统，以将CO2直接捕获和转换为乙醇。该系统由沉积在石墨烯上的天然纤维素和一种新的六角钴纳米片催化剂组成，提供了高导电性和多孔聚合物网络，其中两个组件在直接捕获和电动二氧化碳中合作起作用。富含羟基的无定形纤维素可以以碱催化的亚稳态半碳酸盐的形式捕获CO2。这些亚稳态的半碳酸盐可以在pH变化或轻轻加热后可逆地释放二氧化碳，从而提供了一种能节能的二氧化碳捕获和释放方法，这是受光合作用中自然二氧化碳浓度机制的启发。释放的二氧化碳是靠近石墨烯上组装并集成到纤维素膜中的稳健钴纳米片催化剂的邻近，该催化剂可作为工作电极起作用，以执行CO2的选择性电降低至C2产物。工作流程系统将被证明是一种工程方法，可以将CO2直接捕获和转换为Air作为原料。 The study will offer not only a new design concept on cellulose processing method and new fundamental knowledge on the cobalt nanosheet-promoted C-C coupling in the CO2 reduction reaction, but also an energy-efficient engineering solution to direct CO2 capture and conversion.The portion of this project that will be completed at Brown University is jointly funded by the Electrochemical Systems Program and the Established Program to Stimulate Competitive Research (EPSCoR).This award反映了NSF的法定任务，并使用基金会的知识分子优点和更广泛的影响审查标准来评估值得支持。