Polymer-Protein Hybrid Materials for the Selective Capture of Water Pollutants

在这个由化学系高分子、超分子和纳米化学项目资助的项目中，Matthew B教授。加州大学伯克利分校的弗朗西斯正在合成用于去除水中污染物的新材料。这种新材料是通过将蛋白质附着在聚合物载体上而构建的。由于蛋白质与剧毒物质结合，因此所得的混合材料可用于去除饮用水中的污染物，如多氯联苯，雌激素或其他有毒有机化学品。在这个项目中，正在开发程序来更精确地控制蛋白质和聚合物的附着方式。然后进行进一步的研究，以确定所产生的材料与各种污染物的结合程度，这些污染物已被证明难以从水中去除。这项工作通过应对公共卫生挑战、提高制造过程的安全性以及帮助修复环境污染场地，对我们解决困难的环境问题的能力产生了广泛的影响。这项工作通过一个结合化学、生物学和材料科学多个领域知识的项目，对未来科学家的培训产生了进一步广泛的影响。在这项研究中，杂交材料组成的蛋白质连接到聚合物支持正在建设。蛋白质在结合复杂环境样本中剧毒物种的能力方面是无与伦比的。为了将它们用于修复目的，需要新的合成方法来将多肽与聚合物材料结合，使得所得物质可以促进回收并提高稳定性。在该项目中，正在开发新技术，通过一个有效的化学步骤将聚合物和其他支持物连接到几乎任何所需蛋白质的N末端位置。目前正在研究两种通用的化学改性。在这两种情况下，可以连接单个位置中的所需官能团的单个实例，同时产生稳定的连接。第一种策略涉及由铁氰化物离子促进的化学选择性氧化偶联反应，而第二种策略利用吡啶-2-甲醛（P2CA）衍生物与N-末端氨基酸之间的高选择性反应形成4-咪唑烷酮。这两种策略已经被证明是有用的引入感兴趣的功能基团的模型蛋白质在良好的产量。该项目是建立在早期的结果（1）开发新的偶联剂和条件，以实现更高水平的反应性;（2）确定氨基酸序列对反应性的影响，使用组合肽库;和（3）确认观察到的反应模式，通过连接蛋白质和进化的类肽配体，可以结合难以去除的污染物廉价的聚合物支持。这些新的方法正在测试多氯联苯，雌激素和其他有毒有机污染物通常发现在饮用水源。这些制剂的重金属结合型也在生产中。

In this project funded by the Macromolecular, Supramolecular and Nanochemistry Program in the Chemistry Division, Professor Matthew B. Francis of the University of California, Berkeley, is synthesizing new materials for use in removing pollutants from water. The new materials are constructed by attaching proteins to polymer supports. Since proteins bind to highly toxic substances, the resulting hybrid materials can be used to remove pollutants such as PCBs, estrogens or other toxic organic chemicals from drinking water. In this project, procedures are being developed to more precisely control the ways that the protein and polymer are attached. Further studies are then carried out to determine how well the resulting materials bind to various pollutants that have proven difficult to remove from water. The work is having a broad impact on our ability to tackle difficult environmental problems by addressing challenges to public health, improving the safety of manufacturing processes, and helping to remedy environmental contamination sites. The work is having a further broad impact on the training of future scientists through a project that combines knowledge from multiple fields in chemistry, biology and materials science. In this research, hybrid materials consisting of proteins attached to polymeric supports are being constructed. Proteins are unrivaled in their ability to bind highly toxic species in complex environmental samples. To use them for remediation purposes, new synthetic methods are needed to wed polypeptides with polymeric materials in such a way that the resultant substances can facilitate recovery and improve stability. In this project, new techniques to attach polymers and other supports to the N-terminal position of virtually any desired protein in a single, efficient chemical step are being developed. Two versatile chemical modifications are being studied. In both of these, a single instance of a desired functional group in a single location can be attached while producing stable linkages. The first strategy involves a chemoselective oxidative coupling reaction promoted by ferricyanide ion, while the second exploits the highly-selective reaction between pyridine-2-carboxaldehyde (P2CA) derivatives and N-terminal amino acids to form 4-imidazolidinones. Both strategies have already proven useful for the introduction of interesting functional groups on model proteins in good yields. This project is building on the earlier results by (1) developing new coupling agents and conditions to achieve increased levels of reactivity; (2) determining the effects of amino acid sequence on reactivity using combinatorial peptides libraries; and (3) confirming the observed reactivity patterns by attaching proteins and evolved peptoid ligands that can bind difficult-to-remove pollutants to inexpensive polymer supports. These new methodologies are being tested on PCBs, estrogens, and other toxic organic pollutants commonly found in drinking water sources. Heavy metal-binding versions of these agents are also being produced.