近红外二区硫系银量子点制备方法及癌症诊疗应用研究进展

doi:10.6023/A24060181

化学学报 ›› 2024, Vol. 82 ›› Issue (9): 1001-1012.DOI: 10.6023/A24060181 上一篇

综述

近红外二区硫系银量子点制备方法及癌症诊疗应用研究进展

刘童^a, 皮慧慧^b, 陈冰昆^b^,^*(), 张小玲^a^,^*()

a 北京理工大学化学与化工学院北京 100081
b 北京理工大学光电学院北京 100081

投稿日期:2024-06-03 发布日期:2024-07-22

作者简介:

刘童, 2022年北京理工大学在读硕士研究生, 主要从事基于肿瘤诊疗近红外二区硫系银量子点的制备与应用研究.

皮慧慧, 2022年北京理工大学在读博士研究生, 主要从事基于硫系银量子点光电探测器的制备与应用研究.

陈冰昆, 博士, 北京理工大学光电学院长聘副教授/特别研究员, 博士生导师. 主要从事光电功能材料及其在发光、显示等领域应用研究工作. 2013年在北京理工大学取得博士学位. 入选2014年度“香江学者”研究计划, 于2014~2016年在香港城市大学功能光子学研究中心开展为期两年的博士后研究. 发表SCI论文40余篇, 他引1600余次, 单篇最高引用超400次. 相关研究成果发表在材料、化学、物理化学、光学、纳米等多学科领域国际知名期刊上, 如Adv. Mater., Adv. Funct. Mater., Chem. Mater., Adv. Opt. Mater.等学术杂志. 目前担任光学、纳米、材料领域多个国际知名期刊同行评阅人, MRL期刊青年编委等职务. 获得2018年北京市科学技术奖二等奖.

张小玲, 博士, 北京理工大学化学与化工学院教授, 博士生导师. 主要从事新型光学探针及化学生物传感和环境友好型氟化物等研究工作. 在Angew. Chem.、Anal. Chem.、Chem. Commun.、Biosensors and Bioelectronics、JMC B、Sensors & Actuators: B. Chem等期刊发表学术论文200余篇, 授权国家发明专利10余项, 以主持人或主要完成人获省部级教学成果二等奖2项, 国家技术发明二等奖1项, 省部级科技成果一等奖2项、二等奖3项.

基金资助:
国家自然科学基金(22174008); 国家自然科学基金(22177013); 国家自然科学基金(21974009); 国家自然科学基金(22274010); 基础加强领域基金(2021-JCJQ-2JJ-XXXX); 陕西省人工结构功能材料与器件重点实验室开放基金(AFMD-KFJJ-22102)

Research Progress on the Preparation Method of NIR-II Silver Chalcogenide Quantum Dots and Its Application in Cancer Diagnosis and Treatment

Tong Liu^a, Huihui Pi^b, Bingkun Chen^b,*(), Xiaoling Zhang^a,*()

a School of Chemistry and Chemical Engineering, Beijing Insititute of Technology, Beijing 100081
b School of Optics and Photonics, Beijing Insititute of Technology, Beijing 100081

Received:2024-06-03 Published:2024-07-22
Contact: *E-mail: chenbk@bit.edu.cn;zhangxl@bit.edu.cn
Supported by:
National Natural Science Foundation of China(22174008); National Natural Science Foundation of China(22177013); National Natural Science Foundation of China(21974009); National Natural Science Foundation of China(22274010); Foundation Enhancement Program(2021-JCJQ-2JJ-XXXX); Fundamental Research Funds of Shaanxi Key Laboratory of Artificially-Structured Functional Materials and Devices(AFMD-KFJJ-22102)

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摘要/Abstract

发展新型早期诊断和准确治疗技术是癌症领域重要研究方向. 近红外二区(NIR-II, 1000~1700 nm)荧光成像技术具有组织散射弱与自身荧光低等特点, 因其组织穿透深、空间分辨率好、信噪比高而受到广泛关注. 作为一类NIR-II探针, 硫系银量子点具有可调节的发光性质和良好的生物相容性, 不仅能够用于NIR-II荧光成像, 而且具有实现磁共振成像、计算机断层扫描等多种成像方式以及光致发热等治疗功能的潜力, 有望为癌症诊断和治疗提供新的解决方案. 本文综述了硫系银量子点的分类、NIR-II碲化银量子点的制备及其在肿瘤诊疗方面应用的最新进展, 重点归纳总结了近十年硫系银量子点的研究进展, 并展望了此类多功能NIR-II纳米探针面临的挑战和机遇.

关键词: 近红外二区, 癌症诊疗, 硫系银量子点, 碲化银量子点, 纳米荧光探针

With the increasing number of cancer-related deaths year by year, the development of new early diagnosis and precise treatment techniques has become a crucial research topic in the field of oncology. Fluorescence imaging, as a commonly used diagnostic method for cancer, offers advantages such as non-ionizing radiation and high sensitivity. Compared to traditional visible region and the first near-infrared window imaging technologies, the second near-infrared window (NIR-II, 1000~1700 nm) fluorescence imaging technology presents characteristics of weak tissue scattering and low autofluorescence. Due to its deep tissue penetration, good spatial resolution, and high signal to noise ratio, it has attracted widespread attention. In recent years, a considerable amount of probes operating in NIR-II have been consistently under development. Quantum dots, as a type of nanoprobes, are influenced by the quantum confinement effect, providing tunable luminescent properties that allow absorption and emission wavelengths to span from the visible region to NIR-II. Silver chalcogenide quantum dots, as a low-toxicity type of quantum dots, exhibit excellent biocompatibility. Different methods have been developed to prepare silver chalcogenide quantum dots, including binary and ternary quantum dots, with emission spectra covering the entire range from 350 to 1700 nm. Silver chalcogenide quantum dots not only find applications in NIR-II fluorescence imaging but also hold potential for various imaging modalities such as magnetic resonance imaging, computed tomography, as well as therapeutic functions like photothermal therapy. They can serve as multifunctional biological probes for biological systems, providing innovative approaches for cancer diagnosis and therapy. This article reviews the classification of silver chalcogenide quantum dots, the preparation of NIR-II Ag₂Te quantum dots and the latest advancements in their application in tumor diagnosis and treatment. It outlines the advancements made in the study of silver chalcogenide quantum dots in the last ten years, emphasizing the obstacles and possibilities encountered in the development of these versatile NIR-II nanoprobes.

Key words: the second near-infrared window, cancer diagnosis and treatment, silver chalcogenide quantum dots, Ag₂Te quantum dots, nano-fluorescence probe

引用此文

刘童, 皮慧慧, 陈冰昆, 张小玲. 近红外二区硫系银量子点制备方法及癌症诊疗应用研究进展[J]. 化学学报, 2024, 82(9): 1001-1012.

Tong Liu, Huihui Pi, Bingkun Chen, Xiaoling Zhang. Research Progress on the Preparation Method of NIR-II Silver Chalcogenide Quantum Dots and Its Application in Cancer Diagnosis and Treatment[J]. Acta Chimica Sinica, 2024, 82(9): 1001-1012.

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图/表 9

图1. (a) 荧光成像中光与生物组织的相互作用种类. (b) 水的紫外-可见-近红外吸收光谱. (c) 不同生物组织以及组织分散混合后的散射系数在400~1700 nm范围内与波长关系曲线. (d) 808 nm激发下小鼠离体组织: 心脏(蓝色)、脾脏(红色)和肝脏(黑色)的自身荧光光谱[6]. (e) 可见光以及近红外光在生物组织内穿透深度示意图及量子点结构示意图

Figure 1. (a) Illustration of interactions between light and biological tissue in fluorescence imaging. (b) Ultraviolet-visible-near-infrared absorption spectrum of water. (c) The scattering coefficients curve of different biological tissues and tissues dispersed and mixed with wavelength in the range of 400~1700 nm. (d) Autofluorescence spectra of ex vivo mouse heart tissues (blue), spleen (red), and mouse liver (black) under 808 nm excitation[6]. Copyright 2020 American Chemical Society. (e) The schematic illustration of the penetration depth of the light and structure of quantum dots

NIR-II 材料	优点	缺点
有机小分子	生物相容性高、代谢速率快、分辨率好	光稳定性和水溶性差
共轭聚合物	荧光亮度高、光稳定性好、生物相容性好、水分散性好	激发和发射波长受限
稀土纳米颗粒	发射光谱窄、发射效率高、低光漂白	存在生物毒性隐患、水溶性低
碳纳米管	良好的耐光性	激发强度高、量子产率低
传统量子点	发射光谱窄、激发光谱宽、光学性质稳定、荧光寿命长	毒性高(含重金属元素Cd和Pb)

表1. NIR-II纳米探针优缺点对比[18]

Table 1. Comparison of advantages and disadvantages of NIR-II nanoprobes[18]

图2. (a) 硫系银量子点的发射波长范围. (b) α-Ag2S、(c) β-Ag2Se和(d) β-Ag2Te的晶体结构

Figure 2. (a) Emission wavelength range of silver chalcogenide QDs. Crystalline structure of (b) α-Ag2S, (c) β-Ag2Se and (d) β-Ag2Te

图3. 化学合成中调控量子点尺寸的方法. (a) 有机相中利用三烷基膦调控量子点尺寸[32]. (b) 有机相中通过硫醇蚀刻法调控量子点尺寸[53]. (c) 水相中通过阳离子交换策略调控量子点尺寸[54]

Figure 3. Size control methods of silver chalcogenide quantum dots in chemical synthesis. (a) Controlling quantum dot size via trialkylphosphine-induced ripening in organic phase[32]. (b) Controlling quantum dot size via thiolate etching route in organic phase[53]. (c) Controlling quantum dot size via cation exchanging in aqueous phase[54]. Copyright 2013, 2021, 2022 American Chemical Society

材料	配体	反应温度/℃	发射峰波长/nm	参考
Ag₂S	MPA	145	1221	[60]
Ag₂S	GSH	20	724	[66]
Ag₂S	BSA	37	840	[67]
Ag₂S	HSA	55	1060	[68]
Ag₂S	mPEG-SH	90	1050	[69]
Ag₂S	TAA	r.t.	1250	[70]
Ag₂S	AgBP2	r.t.	1072	[71]
Ag₂Se	GSH	90	820	[61]
Ag₂Se	BSA	55	850	[72]
Ag₂Te	GSH	r.t.	1060	[73]
Ag₂Te	PMAC	r.t.	1068	[40]
Ag₂Te	BSA	r.t.	1050	[64]
Ag₂Te	NAC	r.t.	1160	[73]
Ag₂Te	BSA	r.t.	1050	[26]

表2. 水相合成硫系银量子点制备条件

Table 2. Conditions for preparation of silver chalcogenide quantum dots in aqueous phase

图4. 提高量子点PL QY的策略. (a), (b) 稀土元素掺杂[77]. (c), (d) 过渡金属掺杂[79]. (e), (f) 形成核-壳结构[81]

Figure 4. Strategies to enhance the PL QY of quantum dots. (a), (b) Rare earth element doping[77]. Copyright 2022 Wiley-VCH GmbH. (c), (d) Transition metal doping[79]. Copyright 2023 Elsevier B.V. (e), (f) Core-shell structure growing[81]. Copyright 2020 Small

材料	壳层材料	尺寸/nm	发射峰波长/nm	半峰宽/nm	最大QY/%	参考
Ag₂S@AgCl	AgCl	12.3±1.0	1200＋	150	10.7	[85]
Ag₂S@Cap	Captopril (Cap)	3.89	1005	300		[90]
Ag₂S@ZnS	ZnS	3.4	857	90	5.3	[91]
Ag₂Se@ZnSe	ZnSe	2.0	830~940	20	42	[92]
Ag₂Se@Ag₂S	Ag₂S	4.1~5.4	987~1030	60~70	24.3	[93]
Ag₂Te@ZnS	ZnS	3.04	1042~1120	300	5.6	[54]
Ag₂Te@Ag₂S	Ag₂S	4.89±0.10	1300	200	4.3	[81]
Ag₂Te@Ag₂S	Ag₂S	3.86±0.03	1300	200		[79]
Ag₂Te@Ag₂Se	Ag₂Se	5.4±1.2	1550	400	0.13	[84]
ZnAgInTe₂@ZnS	ZnS	16.93	1090	200	25.2	[44]

表3. 核-壳结构硫系银量子点汇总表

Table 3. Summary of core-shell structure silver chalcogenide quantum dots

图5. 硫系银量子点在癌症诊断中的应用. (a) H2O2活化NIR-II荧光Ag/Ag2S JNPs的机理和应用示意图[70]. (b) L-/D-Ag2S量子点体内NIR-II成像. (c) 不同时间点静脉注射手性Ag2S QDs后的活体小鼠体内NIR-II荧光图像[101]. (d) 小鼠口服BSA-Ag2Te QDs后不同时间点胃肠道的活体CT成像[26]. (e) 纳米生物探针制备及应用示意图. (f) 注射PQDs、PPQDs和CPQDs的4T1荷瘤小鼠体内NIR-II FL成像, 时间为48 h. 白色和绿色虚线圈分别表示肿瘤和正常组织区域[102]

Figure 5. Application of silver-based quantum dots in cancer diagnosis. (a) Schematic illustration of the mechanism and applications of Ag/Ag2S JNPs with H2O2-activated NIR-II fluorescence[70]. Copyright 2021 American Chemical Society. (b) Scheme of in vivo NIR-II imaging with L-/D-Ag2S QDs. (c) Representative NIR-II fluorescence images of living mice after i.v. injection of chiral Ag2S QDs at different timepoints[101]. Copyright 2022 Elsevier. (d) In vivo CT imaging of gastrointestinal tract in Kunming mice at diverse time points after oral injection of BSA-Ag2Te QDs[26]. Copyright 2022 American Chemical Society. (e) Schematic illustration of the nanobioprobe preparation and application. (f) In vivo NIR-II FL imaging of 4T1 tumor-bearing mice injected with PQDs, PPQDs, and CPQDs over the course of 48 h. The white and green dashed circles indicate tumor and normal tissue areas, respectively[102]. Copyright 2019 WILEY-VCH

图6. 硫系银量子点用于癌症诊疗一体化. (a) Ag2S-PAsp (DOX)-cRGDNPs的合成示意图及光化疗增强免疫疗法的抗肿瘤应用. (b) A-P-cRGD NPs对MDA-MB-231荷瘤小鼠的光化学治疗作用[110]. (c) 基于Ag2Se@BSA-DOX-RGD量子点, 结合荧光/光声(FL/PA)成像和靶向化疗/光热治疗建立的一体化治疗纳米平台示意图[72]. (d) 可排泄的超小Ag2Te量子点的制备过程及其在CT成像引导光子肿瘤热疗中的潜在治疗性能示意图. (e) 光子肿瘤热疗[64]

Figure 6. Application of silver-based quantum dots in integration of diagnosis and treatment. (a) Schematic diagram showing the synthesis of Ag2S-PAsp (DOX)-cRGD nanoparticles and the antitumor application of photochemotherapy-enhanced immunotherapy. (b) Photochemotherapy of the A-P-cRGD NPs in MDA-MB-231 tumor-bearing mice[110]. Copyright 2021 Elsevier. (c) Schematic representation of the all-in-one theranostic nanoplatform based on Ag2Se@BSA-DOX-RGD QDs and established by the integration of fluorescence/photoacoustic (FL/PA) imaging and targeted chemo/photothermal therapy[72]. Copyright 2020 Royal Society of Chemistry. (d) Schematic showing the preparation process of excretable ultrasmall Ag2Te QDs and Their Underlying Theranostic Performances of CT Imaging-Guided Photonic Tumor Hyperthermia. (e) Photonic tumor Hyperthermia as enabled by Ag2Te QDs[64]. Copyright 2021 American Chemical Society

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近红外二区硫系银量子点制备方法及癌症诊疗应用研究进展

Research Progress on the Preparation Method of NIR-II Silver Chalcogenide Quantum Dots and Its Application in Cancer Diagnosis and Treatment

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