Collaborative Research: Development and Fundamental Studies of N2-absorbing, Iron-phosphine-containing Polymers for Pressure Swing Purification of Natural Gas

天然气是美国重要的能源。然而，美国的一些天然气储备被氮气污染到必须在使用前去除污染物的程度。在化学系大分子，超分子和纳米化学项目的支持下，太平洋大学的Gohdes博士和俄勒冈州大学的泰勒博士将分子化学与聚合物科学协同结合，设计和合成新型金属模板聚合物（MTP），这将有助于天然气净化的长寿命吸收剂。从该项目中获得的基础知识在催化和传感器设计等其他重要领域具有更广泛的科学意义。从事该项目的本科生和研究生接受实验设计和广泛的合成和分析技术培训。该项目培养学生成为STEM创新的未来领导者。该项目还通过令人兴奋的工具对STEM教育工作者的培训产生了广泛的影响，例如关于非正式科学教育（伊势）的夏季研讨会，对科学教育感兴趣的学生在科学博物馆等场所学习与公众有效沟通的技术。UO的泰勒实验室先前的工作表明，水溶性反式-Fe（P2）2（X）（Cl）型络合物（X = Cl，H; P2 =水溶性双齿膦）可以在适合于变压分离过程的条件下成功地可逆地结合氮气。在这个项目中，Gohdes博士和泰勒博士的目标是通过将氮结合Fe（II）复合物封装在聚合物基质中，在氮结合基序周围形成MTP，来提高氮结合Fe（II）复合物的稳定性。增强氮结合复合物稳定性的另一种方法是用大环四齿膦取代二齿膦。这些小组合作进行研究，以研究铁络合物和MTP的氮结合反应的热力学和动力学。对聚合物的性质如何影响金属中心的固有反应性的基本理解对于下一代氮吸收材料的设计和优化是重要的。

Natural gas is an important source of energy in the United States. However, some of the U.S. natural gas reserves are contaminated with nitrogen gas to the extent that it is necessary to remove the contaminant before it is used. Under the support of the Macromolecular, Supramolecular and Nanochemistry Program in the Division of Chemistry, Dr. Gohdes at Pacific University and Dr. Tyler at the University of Oregon combine molecular chemistry synergistically with polymer science to design and synthesize novel metal-templated polymers (MTPs) that will be useful as long-lived absorbents for the purification of natural gas. The fundamental knowledge gained from this project has broader scientific implications in other important areas such as catalysis and sensor design. Undergraduate and graduate students working on this project receive training in experimental design and a broad array of synthetic and analytical techniques. This project prepares students to become future leaders of innovation in STEM. This project also has extensive impact in the training of STEM educators through exciting vehicles such as a summer workshop on Informal Science Education (ISE) where students interested in science education learn techniques for effectively communicating with the public in venues such as science museums. Prior work in the Tyler lab at the UO showed that water-soluble trans-Fe(P2)2(X)(Cl)-type complexes (X = Cl, H; P2 = a water-soluble bidentate phosphine) can successfully bind nitrogen gas reversibly under conditions suitable for a pressure-swing separation process. In this project, Dr. Gohdes and Dr. Tyler aim to enhance the stability of the nitrogen binding Fe(II) complexes by encapsulating them in a polymer matrix, forming MTPs around the nitrogen binding motif. Another approach to enhance stability of the nitrogen binding complexes is by replacing the bidentate phosphines with macrocyclic, tetradentate phosphines. These groups collaboratively perform research to study the thermodynamics and kinetics of the nitrogen-binding reactions of the iron complexes and MTPs. A fundamental understanding of how the properties of the polymer affect the intrinsic reactivity of the metal center is important for the design and optimization of the next generation nitrogen-absorbing materials.