Using mixed metal clusters in the reductive synthesis of doped ZnO nanocrystals

使用混合金属簇还原合成掺杂 ZnO 纳米晶

• 批准号: 9057070
• 负责人: Emily Tsui
• 金额: $ 5.61万
• 依托单位: UNIVERSITY OF WASHINGTON
• 依托单位国家: 美国
• 财政年份: 2014
• 资助国家: 美国
• 起止时间: 2014-05-21 至 2017-05-20
• 项目状态: 已结题
• 来源: https://reporter.nih.gov/project-details/9057070
• 关键词: Acids; Address; Adsorption; Affect; Anions; Behavior; Biological; Biological Assay; Biosensing Techniques; Biotechnology; Blinking; Cations; Chemicals; Complex; Detection; Development; Diagnosis; Diagnostic; Disease; Effectiveness; Electronics; Elements; Environment; Event; Fluorescence; Foundations; Goals; Growth; Health; Health Care Costs; Image; In Situ; Investigation; Ions; Lanthanoid Series Elements; Ligands; Light; Location; Magnetism; Malignant Neoplasms; Metals; Methodology; Methods; Molecular; Morphology; Nanostructures; Optics; Preparation; Property; Public Health; Quantum Dots; Research; Research Proposals; Route; Salts; Semiconductors; Site; Solvents; Source; Statistical Distributions; Structure; Surface; Techniques; Technology; Temperature; Testing; Therapeutic; Universities; Washington; Work; Zinc; Zinc Cluster; Zinc Oxide; absorption; base; bioimaging; carboxylate; density; design; electric field; fluorescence imaging; human disease; improved; luminescence; magnetic field; metal complex; nanocrystal; nanoscale; novel; novel strategies; physical property; pressure; segregation; small molecule; tool

DESCRIPTION (provided by applicant): The development of new tools for early disease detection and diagnosis is essential to improving public health and lowering healthcare costs. Semiconductor nanocrystals, also known as quantum dots, display optical properties that give them enormous potential in the fields of fluorescence imaging, biosensing, and diagnostics. To advance the effectiveness of nanocrystals in these applications, however, the range of their physical properties must be broadened to include: 1) tuning of fluorescence emission and increased lifetimes 2) sensitivity to electric or magnetic fields and 3) suppression of blinking. One current approach has been the incorporation of metal impurities in the crystal lattice, or doping. Doped nanocrystals comprise a relatively unexplored field, although in recent years nanocrystals with Mn2+, Cu2+, and lanthanide dopants have been studied for their unique optical and magnetic properties. Controlling the amount and location of dopant incorporation within the nanocrystal is important for controlling these new physical properties. Unfortunately, this level o synthetic control has been challenging to achieve, and the mechanisms of dopant incorporation in nanocrystals are still not completely understood. The overall objective of the proposed research is to develop new synthetic methods for doped zinc oxide (ZnO) nanocrystals with improved control over dopant density and distribution. Specifically, this proposal describes the design and synthesis of mixed metal carboxylate-supported multinuclear zinc clusters with coordinated oxometallate ligands as soluble single-source precursors of doped ZnO nanocrystals. The synthesis of these clusters affords the opportunity to study solution-state cluster degradation and aggregation of multinuclear zinc complexes that may serve as intermediates for nucleation clusters. A second aspect of this research plan is to develop a novel approach for the synthesis of doped nanocrystals based upon in situ reduction of oxometallate anions during ZnO lattice growth. With this approach, different nucleation and growth dynamics will be observed that may afford novel and spectroscopically unique nanostructures. These results will allow the design of different types of doped nanocrystals that target specific optical and magnetic properties. The broad, long-term goal of the proposed project is to provide access to these materials to expand the chemical toolkit available for biomedical applications.

描述（由申请人提供）：开发用于早期疾病检测和诊断的新工具对于改善公共卫生和降低医疗成本至关重要。半导体纳米晶体，也被称为量子点，显示出的光学特性使它们在荧光成像、生物传感和诊断领域具有巨大的潜力。然而，为了提高纳米晶体在这些应用中的有效性，必须拓宽其物理性质的范围，以包括：1）荧光发射的调谐和增加的寿命2）对电场或磁场的敏感性和3）闪烁的抑制。目前的一种方法是在晶格中掺入金属杂质或掺杂。 掺杂的纳米晶体包括相对未开发的领域，尽管近年来已经研究了具有Mn 2+、Cu 2+和镧系元素掺杂剂的纳米晶体的独特光学和磁性。控制掺杂剂掺入到掺杂剂中的量和位置对于控制这些新的物理性质是重要的。不幸的是，这种水平的合成控制一直是具有挑战性的实现，掺杂剂掺入纳米晶体的机制仍然没有完全理解。 提出的研究的总体目标是开发新的掺杂氧化锌（ZnO）纳米晶体的合成方法，改善掺杂剂的密度和分布的控制。具体而言，该提案描述了混合金属羧酸盐支持的多核锌簇的设计和合成与协调的金属氧酸盐配体作为可溶性单源前体的掺杂ZnO纳米晶体。这些簇的合成提供了机会，研究溶液状态的簇降解和聚集的多核锌配合物，可以作为成核簇的中间体。本研究计划的第二个方面是开发一种新的方法，用于掺杂的纳米晶体的基础上原位还原的金属氧酸盐阴离子在ZnO晶格生长。通过这种方法，将观察到不同的成核和生长动力学，可以提供新颖的和光谱上独特的纳米结构。这些结果将允许设计不同类型的掺杂纳米晶体，目标是特定的光学和磁性。拟议项目的广泛、长期目标是提供这些材料，以扩大可用于生物医学应用的化学工具包。