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: 8714476
• 负责人: Emily Tsui
• 金额: $ 4.99万
• 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/8714476
• 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 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; Solutions; 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; public health relevance; 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)：开发新的疾病早期检测和诊断工具对于改善公共健康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，具有光学性质，使其在荧光成像、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，必须扩大其物理性质的范围，以包括：1)调节荧光发射和延长寿命；2)对电场或磁场的敏感性；3)抑制闪烁。目前的一种方法是在晶格中掺入金属杂质，或称掺杂。掺杂纳米晶体是一个相对未被开发的领域，尽管近年来，掺杂了Mn2+、Cu2+和La3+的纳米晶体因其独特的光学和磁性而被研究。控制掺杂剂在纳米晶体中的掺杂量和位置对于控制这些新的物理性质非常重要。不幸的是，这一水平的合成控制一直是具有挑战性的，而且掺杂在纳米晶体中的机制仍然不完全清楚。这项研究的总体目标是开发新的掺杂氧化锌纳米晶的合成方法，以改善对掺杂密度和分布的控制。具体地说，这项建议描述了混合金属羧酸盐负载的多核锌簇合物的设计和合成，作为掺杂氧化锌纳米晶的可溶性单源前驱体。这些簇合物的合成为研究多核锌络合物在溶液状态下的降解和聚集提供了机会，多核锌络合物可能是成核簇合物的中间体。这项研究计划的第二个方面是开发一种新的方法来合成掺杂纳米晶，该方法基于氧化锌晶格生长过程中金属氧阴离子的原位还原。通过这种方法，将观察到不同的成核和生长动力学，从而可能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针对特定光学和磁性的掺杂纳米晶。拟议项目的广泛、长期目标是提供获得这些材料的途径，以扩大可用于生物医学应用的化学工具包。