Surface and Interface Mediated Photocoupling Chemistry

描述(申请人提供)：精确控制表面和界面属性的能力在从粘合、生物材料到医疗植入物和微型分析设备的各种应用中至关重要。这些领域的进步需要高度灵敏的生物分析方法和技术，能够提供前所未有的精度和分辨率。表面化学往往是这些技术进步的瓶颈。对表面偶联化学的要求包括精确控制配体的密度、取向和空间呈现，以及最小化非特定相互作用的基质。同样非常理想的是能够适应不同分子结构的配体的偶联化学。能够提供简单性和多功能性的额外好处的技术在临床和工业环境中特别有吸引力。我们发展了一种用于有机分子在固体基质上的共价吸附的光偶联化学。该技术简单、通用性强，可以方便地用高精度、高空间分辨率的外部光进行调制。这种光偶联化学的一个重大挑战是如何精确地控制配体在取向、构象和空间显示方面的呈现。本提案中描述的工作就是为了应对这一挑战。我们的假设是，配体的呈现可以由分子水平上的工程表面和界面控制。以碳水化合物为模型体系，我们将开发控制配体密度和偶联效率的策略(目标1)。配体的构象和呈现将通过结合物理吸附过程来解决，其中配体的构象将由配体与底物(AIM2)的界面相互作用来确定。最后，开发的策略将用于将碳水化合物与纳米材料偶联。这些碳水化合物配体在捕获细菌方面的效率将从配体的呈现和展示方面进行研究(AIM 3)。公共卫生相关性：该项目专注于设计和开发特定用于医疗器械和诊断的功能表面和纳米材料。优化后的材料将特别应用于碳水化合物结构的呈现，因为多糖介导的识别在许多疾病过程中发挥着核心作用，如细菌黏附和炎症过程。所设计的材料随后将应用于生物材料和医疗器械的非血栓形成表面，以及纳米材料对致病细胞的捕获。

DESCRIPTION (provided by applicant): The ability to precisely control surface and interface properties is of paramount importance in applications ranging from adhesion, biomaterials, to medical implants and miniaturized analytical devices. The advance of these fields demands highly sensitive bioanaytical assays and techniques that can offer unprecedented levels of precision and resolution. Surface chemistry is often the bottleneck in the advancement of these techniques. Requirements for surface coupling chemistry include the precise control of the ligand density, orientation and spatial presentation, as well as a matrix that minimizes non-specific interactions. Also highly desirable are coupling chemistries that can accommodate ligands of diverse molecular structures. Techniques that can offer additional benefit of simplicity and versatility are especially attractive in clinical and industrial settings. We have developed a photocoupling chemistry for the covalent attachment of organic molecules on solid substrates. The technique is simple, versatile, and the process can be conveniently modulated by an external light with high precision and spatial resolution. A grand challenge in this photocoupling chemistry is the precise control over the ligand presentation with respect to orientation, conformation, and spatial display. The work described in this proposal is designed to address this challenge. Our hypothesis is that ligand presentation can be controlled by engineering surfaces and interfaces at the molecular level. Using carbohydrates as the model system, we will develop strategies to control the ligand density and the coupling efficiency (AIM 1). The conformation and presentation of the ligand will be addressed by incorporating a physical adsorption process where the ligand conformation will be defined by the interfacial interactions of the ligand with the substrate (AIM 2). Finally, the developed strategies will be employed to couple carbohydrates to nanomaterials. The efficiency of these carbohydrate ligands in capturing bacteria will be studied with regard to the ligand presentation and display (AIM 3). PUBLIC HEALTH RELEVANCE: This project focuses on designing and developing functional surfaces and nanomaterials for specific use in medical devices and diagnostics. The optimized materials will particularly be applied to presentation of carbohydrate structures since glycan-mediated recognition plays a central role in many disease processes, such as bacterial adherence and inflammatory processes. The designed materials will subsequently be applied to nonthrombogenic surfaces for biomaterials and medical devices, and nanomaterial capture of pathogenic cells.