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

在这个由化学学部大分子、超分子和纳米化学项目资助的项目中，加州大学伯克利分校的马修·b·弗朗西斯教授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制成的。由于蛋白质与剧毒物质结合，由此产生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物质。在这个项目中，正在开发更精确地控制蛋白质和聚合物附着方式的程序。然后进行进一步的研究，以确定所得材料与各种已被证明难以从水中去除的污染物的结合程度。这项工作对我们解决困难的环境问题的能力产生了广泛的影响，解决了对公众健康的挑战，提高了制造过程的安全性，并帮助修复了环境污染场所。通过一个结合化学、生物学和材料科学等多个领域知识的项目，这项工作正在对未来科学家的培训产生进一步的广泛影响。在这项研究中，由蛋白质连接到聚合物载体组成的杂交材料正在被构建。蛋白质在复杂环境样品中结合高毒性物种的能力是无与伦比的。为了将多肽用于修复目的，需要新的合成方法将多肽与聚合物材料结合在一起，从而使合成的物质能够促进恢复并提高稳定性。在这个项目中，正在开发一种新技术，可以在一个单一的、有效的化学步骤中将聚合物和其他支撑物连接到几乎任何所需蛋白质的n端位置。目前正在研究两种通用的化学修饰。在这两种方法中，可以在产生稳定连接的同时，在单个位置上连接所需官能团的单个实例。第一种策略是由铁氰化物离子促进的化学选择性氧化偶联反应，第二种策略是利用吡啶-2-甲醛（P2CA）衍生物与n端氨基酸之间的高选择性反应生成4-咪唑烷酮。这两种策略都已被证明是有用的，可以在模型蛋白上以良好的产量引入有趣的官能团。该项目是在早期结果的基础上，通过(1)开发新的偶联剂和条件来提高反应性水平；(2)利用组合肽库测定氨基酸序列对反应性的影响；(3)通过将蛋白质和进化的肽类配体结合到廉价的聚合物载体上，证实观察到的反应模式。这些新方法正在对饮用水源中常见的多氯联苯、雌激素和其他有毒有机污染物进行测试。这些药物的重金属结合版本也正在生产中。

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.