User-controlled Biocatalysis Induces Self-decontamination of Enzyme-based Composites Challenged with Simulant of B. anthracis

在当今社会，人们越来越需要保护人们免受影响健康和福祉的病原体威胁。目前的去污方法是在暴露发生后进行的，通常使用漂白剂、焚烧、光催化或甲醛气体。所有这些都是耗时的，需要大量的资源和人员，对环境不友好，腐蚀性很强，需要大量的剂量才能有效。因此，迫切需要制定能够以经济方式迅速、彻底和成功地解决污染问题的措施。西弗吉尼亚大学化学工程系的PiS Dinu和Wu提议开发基于氯过氧化物酶(CPO)的生物催化剂和光催化剂二氧化钛的自我维持和自去污涂层，能够净化包括蜡状芽胞杆菌(B.ereus)孢子在内的各种病原体(炭疽杆菌的模型)。这种仿生方法利用了CPO附着在二氧化钛纳米材料上，并通过光催化在二氧化钛上原位生成过氧化氢的活性物种。过氧化氢被CPO酶用作局部形成次氯酸的底物，次氯酸是去污剂。这种仿生方法将使生物催化剂的重量解毒许多倍，从而减少运输大量化学品的后勤负担，并消除对环境的破坏。此外，拟议的研究是一个潜在的平台，因为它的成功完成将为未来使用不同特性的酶的鸡尾酒对各种化学和生物制剂进行基于生物催化的去污奠定基础。人们已经注意到设计环境友好型涂层的尝试，这种涂层能够以经济的方式快速和完全地去污包括孢子在内的各种生物制剂，并且不会对广泛的部署造成不必要的后勤负担。Dinu和Wu提议使用纳米二氧化钛材料原位产生过氧化氢。然后，酶-纳米材料的结合物可以被加入到涂料中，生成能够净化吸附在表面的任何物种的涂层。这项研究具有重要意义，因为它的成功完成将带来关于酶-纳米材料偶联物的结构亲和力、结构稳定性和结构功能关系的基础知识。了解酶支架如何通过与二氧化钛等纳米材料的共价或非共价结合来稳定，反过来将有助于理解电子转移的平台和去污途径。这样的平台可以通过对纳米材料或酶的修饰来进一步设计，以调整电子转移性质，并允许用户控制基于生物催化剂的去污染。该项目还提供了教育方面的潜力。拟议研究的内在跨学科性质提供了巨大的机会，可以吸引和整合学生在不同领域的教育经验，包括生物、生物化学、物理、化学和材料科学。由于该项目涉及各行各业的人都感兴趣和关注的生活方面，而且可以用容易理解的术语进行交流，因此推广和公众教育的潜力非常大。

1033266DinuIn today's society, there is a constant growing need to protect people from exposure to pathogen threats that affect health and wellbeing. Current decontamination methods are performed after exposure has occurred, and typically employ bleach, incineration, photocatalysis, or formaldehyde gas. All are time consuming, require significant resources and personnel, are environmentally unfriendly and highly corrosive, and require significant dosages to be effective. Thus, there is a critical need to develop measures that can successfully address contamination rapidly, completely, and in an economical manner. PIs Dinu and Wu of the Chemical Engineering Department at West Virginia University propose to develop self-sustainable and self-decontaminating coatings which are based on biocatalysts of chloroperoxidase (CPO) enzyme and the photocatalyst titanium dioxide, which are capable of decontaminating a large variety of pathogens, including spores of B. cereus (a model for B. anthracis). The biomimetic approach capitalizes upon the attachment of CPO to titanium dioxide nanomaterials, and in situ generation of reactive species of hydrogen peroxide by photocatalysis on the titanium oxide. The peroxide is used by the CPO enzyme as substrate for the local formation of hypochlorous acid, which is the decontaminant. This biomimetic approach would detoxify many times the biocatalyst weight thus reducing the logistical burdens of delivering large amounts of chemicals and eliminating environmental damage. Moreover, the proposed research is a potential platform as its successful completion would lay the foundation for future application of biocatalytic-based decontamination to a variety of chemical and biological agents by using a cocktail of enzyme with different specificities.The broader implications have already been recognized. Attention has been given to attempts to design environmentally friendly coatings that are capable of decontaminating a large variety of biological agents including spores, rapidly and completely, in an economical manner and without imposing an undue logistical burden for widespread deployment. Dinu and Wu propose to use nanomaterials of titanium dioxide for in situ generation of hydrogen peroxide. The enzyme-nanomaterials conjugates could then be incorporated into paint andgenerate coatings capable of decontaminating any species that adsorbs on the surface. The proposed research is significant because its successful completion will lead to fundamental knowledge about structure-affinity, structure-stability, and structure-function relationships for enzyme-nanomaterial conjugates. Understanding how the enzyme scaffolding can bestabilized by covalent or non-covalent association with nanomaterials such as titanium dioxide will in turn lead to understanding the platform for electron transfer and the decontamination pathways. Such a platform can be further engineered by modification of the nanomaterial or of the enzyme to tune the electron transfer properties and allow user-control of the biocatalytic-based decontamination. The project offers potential in education as well. The inherent interdisciplinary nature of the proposed research offers tremendous opportunities for enticing and integrating students with educational experience across diverse areas including biology, biochemistry, physics, chemistry and materials science. As the project involves aspects of life that are of interest and concern to people in many walks of life, and can be communicated in easily understood terms, the outreach and public education potential is very large.