Membrane Recovery of Homogeneous Catalysts (TSE 99-D)

摘要提案编号：CTS-9985552提案类型：对NSF 99-108，NSF/EPA可持续环境计划技术的响应主要研究者：玛丽·雷扎克和哈斯克尔·贝克汉姆所属机构： 格鲁吉亚理工学院均相催化剂的膜回收均相催化剂由于其高反应速率和选择性而用于化学生产。 然而，这些催化剂的回收和再循环是困难的，并产生大量废物（1996年约400万吨）。 常规技术不太适合这种分离。 该研究项目考察了由交联二乙炔官能化聚合物开发的化学稳定膜从水性或非水性反应混合物中选择性回收均相催化剂的能力。如果成功，该技术可以极大地扩展高选择性但通常昂贵的均相催化剂的使用，并显著减少通过常规多相催化体系形成的不期望的副产物的体积。配体催化剂可以用基于两种化合物的扩散速率的差异提供选择性的有机聚合物膜来实现。 基于迁移率的选择性的定制可以通过控制聚合物链的分子运动来实现。 聚合物基质的选择性交联可用于获得这种控制。 将研究通过二乙炔官能度进行局部化学交联的聚合物，以探测该单元防止聚合物溶胀和同时损失选择性而不显著降低所需反渗透剂的传输速率的能力。 将系统地改变样品的交联密度，以评价提出的假设。测量每种渗透剂的溶解度和扩散系数。评价了膜在均相催化剂回收中的性能和回收催化剂的后续活性。

AbstractProposal number: CTS-9985552Proposal type: Response to NSF 99-108, NSF/EPA Technology for a Sustainable Environment ProgramPrincipal investigators: Mary Rezac and Haskell BeckhamAffiliation: Georgia Institute of Technology Membrane Recovery of Homogeneous CatalystsHomogeneous catalysts are employed for chemical production because of their high reaction rates and selectivity. However, recovery and recycle of these catalysts is difficult and produces significant waste (approximately 4 million tons in 1996). Conventional techniques are not well suited to this separation. This research program examines the ability of chemically stable membranes developed from crosslinked diacetylene-functionalized polymers to selectively recover homogeneous catalysts from either aqueous or non-aqueous reaction mixtures. If successful, this technology could greatly expand the use of highly selective but often expensive homogeneous catalysts and dramatically reduce the volume of undesired by-products formed via conventional heterogeneous catalysis systems.The hypothesis of this study is that the separation of an organic product from a metal-ligand catalyst can be achieved with an organic polymer membrane that provides selectivity based on differences in the diffusion rates of the two compounds. Tailoring of mobility-based selectivity can be realized through control of the molecular motion of the polymer chains. Selective crosslinking of the polymer matrix can be used to gain this control. Polymers topochemically crosslinked via a diacetylene functionality will be investigated to probe the ability of this unit to prevent polymer swelling and the concurrent loss of selectivity without markedly reducing transport rates of desired penetrants. The crosslink density of the samples will be systematically varied to evaluate the posed hypothesis. Measurement of the solubility and diffusion coefficient for each penetrant will be made. The performance of the membrane in the recovery of homogeneous catalyst and the subsequent activity of the recovered catalyst are being evaluated.