论文总字数：29441字

摘 要

在过去的几十年中，伴随着纳米技术的快速发展，已成功合成了高质量的镧系元素掺杂上转换纳米粒子（UCNPs）。由于其优异的化学和光学特性，镧系掺杂的上转换纳米粒子（UCNPs）可以显示出独特的上转换光致发光（UCPL），因此引起了人们的广泛关注。由于镧系离子的独特电子构型，在近红外，可见和紫外光谱范围内具有丰富的能级结构。然而，对于UCNP，由于敏化剂（Yb³ ）和活化剂（Er3 ，Tm³ 和Ho³ ）离子的数量有限，仅产生了有限数量的高效上转换激发和发射，并且应用主要集中在人们通过使用UCNP的上转换发光进行成像。最近，越来越多的研究人员开始关注上转换光学性质的调整和多功能UCNP的开发，结合​​亚晶格介导的能量迁移，核心壳结构工程和基于UCNPs的纳米复合材料，大大扩展了纳米复合材料的范围。镧系元素掺杂的UCNPs的应用。与下移发光相比，UCPL在生物应用中展现了其光明的未来，其中多种低能光子（例如近红外（NIR）激发）的顺序吸收由镧系离子的梯状能级实现。（Ln³ ）导致产生更高能量的光子（例如紫外线，可见光）。UCPL具有多种优点，例如尖锐的发射，大的反斯托克斯位移，长的发光寿命和高的光漂白抗性。此外，NIR照射具有较低的光损伤效果，在组织中具有较大的穿透深度，同时可以避免生物样品的自发荧光干扰和光散射现象，从而可以减少背景光并改善信号 - 噪音比。因此，UCNP已成为更适合生物应用的纳米材料。迄今为止，许多科学家一直致力于研究UCNPs的生物应用，包括生物成像，药物释放和特殊表面修饰后的治疗。

关键字：UCNPs（上转换纳米粒子）; UCPL（上转换光致发光）; 镧系离子; 量子点; CD，（碳点）; CW（连续波长）;

Mesoporous modified upconversion nanocrystals for preparation of near-infrared excitation up-conversion nanoprobes

Abstract

In the past decade, with the rapid development of nanotechnology, high quality lanthanide doped upconversion nanoparticles (UCNPs) have been successfully synthesized. Because of its excellent chemical and optical properties, lanthanide doped upconversion nanoparticles (UCNPs) can display unique upconversion photoluminescence (UCPL), which has attracted wide attention. Due to the unique electronic configuration of lanthanide ions, there are abundant energy levels in the near infrared, visible and ultraviolet spectra. However, for UCNP, due to the limited number of sensitizers (Yb3 ) and activators (Tm3 , Er3 , and Ho3 ), only a limited number of highly efficient up-conversion excitation and emission have been generated, and applications are mainly focused on imaging by using up-conversion luminescence of UCNP. Recently, more and more researchers began to pay attention to the upconversion optical properties adjustment and the development of multifunctional UCNP. Combined with sublattice-mediated energy transfer, core-shell structure engineering and UCNPs-based nanocomposites have greatly expanded the scope of nanocomposites. Application of lanthanide doped UCNPs. Compared with down-shifting luminescence, UCPL has a bright future in biological applications. The sequential absorption of many low-energy photons (such as near infrared (NIR) excitation) is realized by ladder levels of lanthanide ions. (Ln3 ) results in higher energy photons (such as ultraviolet and visible light). UCPL has many advantages, such as large anti-Stokes shift, sharp emission, long luminescence lifetime and high photobleaching resistance. In addition, NIR irradiation has a lower light damage effect, a greater penetration depth in tissues, and can avoid spontaneous fluorescence interference and light scattering of biological samples, thus reducing background light and improving signal-to-noise ratio. Therefore, UCNP has become a more suitable nanomaterial for biological applications. So far, many scientists have been working on the biological applications of UCNPs, including bioimaging, drug release and special surface modification therapy.

Key words：UCNPs (upconversion nanoparticles); UCPL (upconversion photoluminescence); lanthanide ions; quantum dots; CD (carbon dots); CW (continuous wavelength);

目录

目录

介孔修饰上转换纳米晶制备近红外激发上转换纳米探针 I

摘要 I

Abstract II

第一章 绪论 1

1.1引言 1

1.2上转换纳米粒子的典型合成 3

1.2.1热分解方法 3

1.2.2水热/溶剂热法 4

1.2.3共沉淀法 5

1.3 上转换纳米粒子的改性策略 6

1.4通过构建核/壳结构来增强上转换光致发光 7

1.5水溶性上转换纳米粒子的合成 9

1.5.1无机表面硅烷化 9

1.5.2有机配体改性方法 10

1.6用于传感的上转换纳米颗粒 12

1.6.1用于阴离子传感的上转换纳米粒子 12

1.6.2用于阳离子传感的上转换纳米粒子 13

1.6.3。用于分子感应的上转换纳米粒子 13

1.6.4用于pH传感的上转换纳米粒子 14

1.6.5用于温度传感上转换纳米粒子 15

1.7 本文研究内容及方法 15

1.7.1 研究内容 15

1.7.2 合成方法 15

第二章 实验部分 17

2.1 实验仪器 17

2.2 实验试剂 17

2.3 实验步骤 18

2.3.1实验主要步骤 18

2.3.2合成纳米粒子 18

第三章 结果与讨论 19

3.1合成条件 19

3.1.1 OA-UCNP的合成条件 19

3.1.2 CD-UCNP的合成条件 21

3.2谱图分析 21

3.2.1所得产物的荧光谱图和文献的荧光谱图的对比 21

3.2.2 NaYF₄: Er,Tm,Yb@SiO₂/CD的合成以及纳米粒子包裹前后的表征 23

3.2.3 XRD谱图的表征 24

3.2.4 TEM谱图的表征 25

第四章 结论与展望 26

参考文献 26

致谢 32

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