Biomimetic and Rubisco-Inspired CO2 Capture from Air

在该项目中，由化学系的化学结构、动力学机制B计划资助，哥伦比亚密苏里州大学化学系的Rainer Glaser教授正在开发用于从空气中可逆捕获二氧化碳的二氧化碳捕获和释放（CCR）系统。这种仿生CCR系统的设计是通过了解二氧化碳在rubisco酶的活性位点的结合而得知的。开发了一种用于农业温室中二氧化碳富集的简单装置，以在田间试验中证明CCR概念。预计未来将用于大规模、分布式的从空气中去除二氧化碳及其随后的永久捕获和储存。该项目提供跨学科培训（机械，结构和计算化学;蛋白质合成和生物材料）。通过在科学传播和科学写作课程中开发“化学是新闻”项目，以指导学生科学过程，科学写作，科学同行评议和职业道德，实现了更广泛的影响。 用小分子模型对二氧化碳捕获反应进行了详细的热力学分析，证明了以rubisco为灵感的小肽仿生物作为二氧化碳释放能量要求低的CCR系统的前景。节能CCR系统的实现需要开发具有相当大的负反应熵的二氧化碳捕获反应。本研究的目标是鉴定具有捕获热化学的小肽，其最适合于有效捕获和能量有效释放。为此，合成了游离和固定化四肽的文库。具体的实验包括（a）二氧化硅颗粒合成和表面官能化，（B）在各种载体上的肽固定，（c）通过光谱学和肽晶体学表征，（d）二氧化碳吸附/解吸的定量测量，和（e）用于二氧化碳富集的简单装置的制造。实验工作伴随着四肽库的理论研究，以确定热化学和动力学的二氧化碳除了镁络合的四肽，以评估镁的替代品。

In this project, funded by the Chemical Structure, Dynamic & Mechanism B Program of the Chemistry Division, Professor Rainer Glaser of the Department of Chemistry at the University of Missouri, Columbia is developing carbon dioxide capture and release (CCR) systems for the reversible carbon dioxide capture from air. The design of this biomimetic CCR systems is informed by the understanding of the binding of carbon dioxide in the active site of the enzyme rubisco. A simple device for carbon dioxide enrichment in agricultural greenhouses is developed to demonstrate the CCR concept in a field test. Future use is envisioned for large-scale, distributed carbon dioxide removal from air and its subsequent permanent capture and storage. The project provides cross-disciplinary training (mechanistic, structural and computational chemistry; protein synthesis, and biomaterials). Additional broader impacts are achieved through the development of the "Chemistry is in the News" project in science communication and the scientific writing curriculum to instruct students about the scientific process, scientific writing, scientific peer review, and professional ethics. Detailed thermodynamic analyses performed for the carbon dioxide capture reaction with a small molecule model demonstrates the promise of rubisco-inspired, small peptide biomimetics as CCR systems with low energy requirements for carbon dioxide release. The realization of energy-efficient CCR systems requires the development of carbon dioxide capture reactions with negative reaction entropies of substantial magnitude. It is the goal of this research to identify small peptides with capture thermochemistry most suitable for effective capture and energy-efficient release. For this purpose, libraries of free and immobilized tetrapeptides are synthesized. Specific experiments include (a) silica particle synthesis and surface functionalization,(b) peptide immobilization on various supports,(c) characterization by spectroscopy and by peptide crystallography,(d) quantitative measurements of carbon dioxide sorption/desorption,and (e) the fabrication of a simple device for carbon dioxide enrichment. The experimental effort is accompanied by theoretical studies of the library of tetrapeptides to determine the thermochemistry and the kinetics of the carbon dioxide addition to the magnesium complexed tetrapeptides, to assess alternatives to magnesium.