乳腺癌是威胁女性健康的杀手。作为微创疗法的光热治疗具有高特异性、低侵袭性和时空可控的优点，已有针对乳腺癌治疗开展的临床前研究。目前开发的有机光热制剂（Photothermal Agents，PTA）因π-π堆积存在光稳定性差和在高浓度中易聚集导致荧光减弱等不足，因此亟待开发性能优异且发光稳定的聚集诱导发光（Aggregation Induced Emission，AIE）性质的有机PTA。近红外二区（Near-Infrared-II，NIR-II）荧光成像具有最小的组织自身荧光水平、高灵敏度和更好的空间分辨率的特性，光声成像（Photoacoustic Imaging，PAI）可提供更深入的组织穿透，具有多模成像性能的PTA为复杂的肿瘤微环境提供更多可能。因此，迫切需要开发高性能AIE纳米诊疗剂用于乳腺癌精准治疗。

       本论文通过调控能量在辐射跃迁与非辐射跃迁中的流动，利用不同策略进行分子修饰，从而提高有机PTA的光热性能，构建稳定优异的AIE型纳米诊疗剂，具体内容如下：

（1）通过氟化策略修饰非富勒烯受体Y5-2BO，将苯环扩展为萘环，延长π共轭结构，引入“无障碍”转子三氟甲基，设计合成AIE性质的Y5-2BO-2BTF，增强相邻分子间的静电相互作用，促进吸收波长红移。Y5-2BO-2BTF的非平面构象有限阻止了π-π堆积，在高浓度下荧光不断增强。经聚合物F127包裹形成带负电的球形的Y5-2BO-2BTF NPs，并且在808 nm（0.8 W cm⁻²）激光照射下具有82.94%的高光热转换效率，是Y5-2BO NPs光热转换效率的1.5倍，较ICG有更好的光稳定性。动物实验结果表明，Y5-2BO-2BTF NPs在小鼠乳腺原位瘤模型中光热治疗效果良好，且具有良好的生物安全性。

（2）通过延长侧链调控分子间作用力改变CIPC-2EH共轭基团和改变CIPC-3C₈ 侧链基团修饰合成CIPC-3EH，期待提高摩尔消光系数，CIPC-3EH的摩尔消光系数高达8.0 × 10⁴ cm⁻¹M⁻¹，使其共轭聚合物具有AIE性质，避免完全的平面结构限制其非辐射跃迁。CIPC-3EH是“A-D-A”型结构，紫外吸收证明具有宽的吸收光谱，并且发光可到NIR-II区。经F127包裹CIPC-3EH形成带负电的球形的CIPC-3EH NPs，有利于在体长循环。体外实验证明波长的红移和光热性能的增强，在808 nm（0.8 W cm⁻²）激光照射10 min下，CIPC-3EH NPs最高温度可达60 ℃以上；CIPC-3EH NPs在小鼠乳腺原位瘤模型中实现肿瘤处被动富集，尤其是在脑胶质瘤原位模型中显现出NIR-II LP1500 nm优异的成像效果；在细胞水平，CIPC-3EH NPs在808 nm（0.8 W cm⁻²）激光照射下，在100 μM下可达到约90%的杀伤且在体具有良好的肿瘤杀伤效果，在体安全性良好。

      综上所述，本论文通过两种不同策略构建了高性能的AIE纳米诊疗剂，在乳腺癌精准治疗中取得了良好进展，进一步推进AIE型探针在乳腺癌精准诊断与治疗方面的应用。

Breast cancer is a killer that threatens women's health. As a minimally invasive therapy, photothermal therapy has the advantages of high specificity, low invasiveness and spatio temporal controllability, and preclinical studies have been carried out for the treatment of breast cancer. Currently developed photothermal agents (PTA) have shortcomings such as poor photostability due to π-π deposition and weak fluorescence due to easy aggregation at high concentrations. Therefore, it is urgent to develop organic PTA with excellent performance and stable luminescence with aggregation-induced emission properties. Near-Infrared II (NIR-II) fluorescence imaging has the characteristics of minimum tissue self-fluorescence level, high sensitivity and better spatial resolution, photoacoustic imaging (PAI) can provide deeper tissue penetration. PTAs with multimodal imaging properties offer more possibilities for complex tumor microenvironments. Therefore, there is an urgent need to develop high-performance AIE nanotheranostic agents for the precision treatment of breast cancer.

 

In this paper, by regulating the flow of energy in radiative and non-radiative transitions, molecular modifications were carried out using different strategies, so as to improve the photothermal properties of organic PTA and construct stable and excellent AIE nanotheranostic agents. The specific contents are as follows：

 

(1) The non-fullerene receptor Y5-2BO was modified by fluorination strategy, the benzene ring was extended to naphthalene ring, the π-π conjugated structure was extended, the "barrier-free" rotor trifluoromethyl was introduced, and Y5-2BO-2BTF with AIE properties was designed and synthesized, which enhanced the electrostatic interaction between adjacent molecules and promoted the absorption wavelength redshift. The non-planar conformation of Y5-2BO-2BTF prevents π-π accumulation, and the fluorescence of Y5-2BO-2BTF is enhanced at high concentrations. The negatively charged spherical Y5-2BO-2BTF NPs was formed by polymer F127, and had a high photothermal conversion efficiency of 82.94% under 808 nm (0.8 W cm⁻²) laser irradiation, which was 1.5 times that of Y5-2BO NPs, and had better photostability than ICG. The results of animal experiments show that Y5-2BO-2BTF NPs has good photothermal treatment effect and good biosafety in the mouse model of breast cancer in situ.

(2) The modification of CIPC-3EH by changing the CIPC-2EH conjugated groups and changing the CIPC-3C₈ side chain groups is expected to improve the molar extinction coefficient. The molar extinction coefficient of CIPC-3EH is as high as 8.0 × 10⁴ cm⁻¹M⁻¹, which makes the conjugated polymer with AIE properties. Avoiding a completely flat structure limits its non-radiative transitions. CIPC-3EH is an "A-D-A" type structure with a wide absorption spectrum demonstrated by UV absorption and luminescence up to the NIR-II region. CIPC-3EH is wrapped by F127 to form a negatively charged spherical CIPC-3EH NPs, which is conducive to circulation in the body length. In vitro experiments show that the wavelength redshift and photothermal properties are enhanced. Under 808 nm (0.8 W cm⁻²) laser irradiation for 10 min, the maximum temperature of CIPC-3EH NPs can reach more than 60 ℃. CIPC-3EH NPs can achieve passive enrichment of tumor in mouse breast cancer in situ model, especially in brain glioma in situ model, showing excellent imaging effect of NIR-II LP1500 nm. At the cellular level, CIPC-3EH NPs can achieve about 90% kill at 100 μM under 808 nm (0.8 W cm⁻²) laser irradiation, and has good tumor killing effect in vivo, and with good safety in vivo.

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