CAREER: CAS: Organic Photochemistry for Light-Driven CO2 Capture and Release

职业：CAS：光驱动二氧化碳捕获和释放的有机光化学

• 批准号: 2338206
• 负责人: Richard Liu
• 金额: $ 77万
• 依托单位: Harvard University
• 依托单位国家: 美国
• 项目类别: Continuing Grant
• 财政年份: 2024
• 资助国家: 美国
• 起止时间: 2024-07-01 至 2029-06-30
• 项目状态: 未结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=2338206&HistoricalAwards=false
• 关键词: CAREER; CAS; Organic; Photochemistry; Light

With support from the Chemical Structure, Dynamics & Mechanisms-B (CSDM-B) Program of the Chemistry Division, Richard Liu of the Department of Chemistry and Chemical Biology at Harvard University is developing new classes of photoswitchable organic compounds to enable control of carbon dioxide (CO2) binding and release with visible light. This fundamental knowledge may be used to develop devices that harness energy from sunlight to separate CO2 from emission streams or directly from the atmosphere and then release that captured CO2 on demand for utilization or storage. This project integrates these research goals with educational activities intended to promote broader participation in scientific careers, specifically aimed at engaging K-12 students in the Boston area as well as adult and non-traditional learners. Tools for teaching organic chemistry concepts to blind and low-vision students will also be developed, focusing on topics such as molecular geometry, stereochemistry, and isomerization reactions related to the research aims.Photochromic organic molecules are promising materials for directly light-driven separations, as they may be efficiently switched between two or more isomeric forms that can differ significantly in their chemical properties. The proposed research outlines general schemes for coupling of these optically controlled equilibria to downstream light-independent equilibria involving CO2 uptake into solution. In one mode, new compounds that enter a metastable, highly acidic state upon irradiation will be used for passive capture and on-demand release of CO2. In a second, complementary mode, reversible photobases – a neglected class of compounds with few known examples – will be employed to enable light-triggered capture and gradual passive release. Co-operative mechanisms involving the combination of photoacids or photobases with traditional amine sorbents will also be explored. For each class of compounds, in situ spectrophotometry, pH and CO2 measurement, and ultrafast spectroscopy will be used to characterize key photochemical mechanisms. The thermodynamic requirements for effective photoswitching will be revealed through systematic synthesis and evaluation of photoswitches.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.

在化学司的化学结构，动力学B（CSDM-B）计划的支持下，哈佛大学化学与化学生物学系的理查德·刘（Richard Liu）正在开发新的可拍照有机化合物的新类别，以控制二氧化碳（CO2）的二氧化碳（CO2）结合和可见光的释放。这种基本知识可用于开发从阳光到发射流分开或直接与大气分开的设备，然后释放按需捕获二氧化碳的使用或储存。该项目将这些研究目标与旨在促进科学职业的更广泛参与的教育活动相结合，专门旨在吸引波士顿地区的K-12学生以及成人和非传统学习者。还将开发用于盲目和低视觉学生的有机化学概念的工具，重点关注与研究目的相关的分子几何，立体化学和异构化反应等主题。在两种形式之间可以有效地切换，可以在两种或更相关的形式之间有效地切换，从而有效地切换了它们，可以在化学范围内有效地切换，从而有效地在化学上有明显的属性。拟议的研究概述了这些光学控制的等效性脑耦合到下游光无依赖性等效性脑的一般方案，涉及二氧化碳吸收到溶液中。在一种模式下，辐射后进入亚稳态的高度酸性状态的新化合物将用于被动捕获和按需释放CO2。在第二个完整的模式下，将使用可逆光剂 - 很少有已知示例的负类化合物 - 将采用光触发的捕获和等级被动释放。还将探索合作机制，涉及光子或光剂与传统胺吸附剂的组合。对于每类化合物，原位分光光度法，pH和CO2测量以及超快光谱法将用于表征关键的光化学机制。有效的照片处理的热力学要求将通过系统的综合和对照片开关的评估来揭示。该奖项反映了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评估标准，通过评估被认为是宝贵的支持。