Recent progress of heterojunction materials for tumor diagnosis and treatment
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摘要: 癌症是目前全球范围内引起死亡的主要疾病之一，受到人们的高度重视。然而传统的癌症治疗方法仍存在许多缺陷，严重影响了癌症治疗效果并给患者带来了许多不利影响。随着纳米材料的发展，光动力疗法(PDT)和光热疗法(PTT)等新型治疗方法有效弥补了传统治疗方法的不足。其中，将不同成分的纳米半导体材料组合成一个纳米结构的异质结在光动力疗法和光热疗法上有着优异的表现。异质结材料因其特有光学特性和结构设计性，在催化、检测、多模态成像和肿瘤的协同治疗领域中有很大的应用潜力。本文根据结构分类对不同种类异质结的原理进行了大致介绍，并对近年来异质结材料在肿瘤的单重治疗、协同治疗与诊疗一体化中的研究进展进行了系统性的综述，最后对异质结材料在癌症诊断治疗领域的未来发展方向进行了展望。Abstract: At present, cancer is one of the major fatal diseases worldwide, and traditional treatment methods have many drawbacks. New therapeutic methods such as photodynamic therapy (PDT) and photothermal therapy (PTT) have effectively made up for the deficiency of traditional therapeutic methods with the development of nanomaterials. Heterojunction which combines nanomaterials of different compositions into a nanostructure exhibits an excellent performance in photodynamic therapy and photothermal therapy. Heterojunction materials have great application potential in the fields of catalysis, detection, multi-modal imaging and collaborative treatment of tumors due to their inherent peculiarities, including magnetic properties, optical properties and structural design. This article systematically reviews the recent progress of heterojunction materials in single tumor therapy, cooperative therapy and the integration of diagnosis and treatment, and the future development direction of heterojunction materials is also prospected.
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Key words:
- heterojunction /
- tumor therapy /
- photothermal therapy /
- synergistic therapy /
- multimodal imaging
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Figure 1. Schematic representation of electron-hole pair separation in different kinds of heterojunctions[51-52] ((a) Single semiconductor and heterojunctions; (b) Conventional type II heterojunctions; (c) p-n heterojunctions; (d) Schottky heterojunctions; (e) Direct Z-type heterojunctions; (f) CNT heterojunctions; (g) Graphene heterojunctions)
CB—Conduction band; VB—Valence band; CNT—Carbon nanotube
图 3 用于光动力治疗的g-C3N4-Au NPs的细胞内活性氧(ROS)的产生检测 ((a)~(b)) 、体外PDT效应 ((c)~(d)) 和体内抗癌效果 ((e)~(i))[95]
Figure 3. Detection of intracellular reactive oxygen species (ROS) production ((a)-(b)), in vitro PDT effects ((c)-(d)) and in vivo anti-cancer effects ((e)-(i)) of g-C3N4–Au NPs for photodynamic therapy[95]
图 4 二维热氧化黄铁矿纳米片(TOPY NSs)的光热治疗的示意图 (a)、靶成像向效果 (b) 和作为PA成像剂效果评估 (c)[101]
Figure 4. Schematic diagram of photothermal therapy (a) and the evaluation of the target imaging effect (b) and the effect used as a PA imaging agent (c) of two-dimensional thermal oxidized pyrite nanosheets (TOPY-PEG NSs)[101]
GSH—Glutathione; GSSG—Ooxidized glutathione; PEG—Polyethylene glycol; NMP—N-methylpyrrolidone)
图 5 替拉帕嗪/纳米粒子@卟啉金属-有机骨架材料(TPZ/UCSs)异质结[111]结构示意图及其在近红外光(NIR)激发PDT和低氧活化化疗联合免疫治疗肿瘤中的应用(a)；NIR光触发组合疗法的示意图 (b)；经过不同处理的CT26荷瘤小鼠中原发性肿瘤 (c) 和远处肿瘤 (d) 的生长曲线；顺铂-AuNRs@SiO2-Avastin@PEI/AE105 NPs[113]化学-光热宫颈癌联合治疗临床诊断设计示意图 (e) 及其光热效果 ((f)~(g))，肿瘤治疗效果图 ((h)~(i)) ;HPT-DOX[115]制备与超声动力及化疗联合抗癌机制的示意图 (j)、超声动力效果 (k)、高分辨TEM图像与元素映射 (l)
Figure 5. Schematic diagram of the structure and the application in NIR-stimulated PDT and hypoxic-activated chemotherapy combined immunotherapy (a) of tirapazamine (TPZ/UCSs) heterojunction[111]; schematic diagram (b) of NIR light-triggered combination therapy of TPZ/UCSs heterojunction; growth curves of primary tumors (c) and distant tumors (d) of CT26 tumor-bearing mice under different treatments; schematic diagram (e) of the clinical diagnosis design of the photothermal-chemotherapy combined cervical cancer treatment, the photothermal effect ((f)-(g)) andthe anticancer effect ((h)-(i)) of cisplatin-AuNRs@SiO2-Avastin@PEI/AE105 NPs[113]; schematic diagram (j) of the preparation process and the sonodynamic-chemotherapy combined anticancer mechanism and the graph of ultrasonic dynamic effect (k), the high-resolution TEM image and element mapping (l) of HPT-DOX [115]
图 6 2D CONs异质结的体内肿瘤治疗及光热疗法(PTT)和I型光动力疗法(PDT)生成机制示意图 (a)、Live/Dead荧光染色图 (b)[117]；BiOI@Bi2S3的异质结纳米颗粒放射/光动力/光热治疗效率增强原理示意图 (c)、肿瘤形貌及H&E染色 (d)、体内PA成像图 (e)[116]
Figure 6. Schematic illustration ofthe in vivo tumor therapy and the generation mechanism of photothermal therapy (PTT) and type I photodynamic therapy (PDT) (a) , live/Dead fluorescence staining diagram of 2D CON (b)[117]; Schematic diagram of RF/photodynamic/photothermal treatment efficiency enhancement principle (c) and the graph of tumor morphology and H&E staining (d) and in vivo PA imaging of BiOI@Bi2S3 heterojunction nanoparticles (e)[116]
COF—Covalent organic framework; CONs—Covalent organic nanosheets; HHTP—2,3,6,7,10,11-hexahydroxytriphenylene; Por—5,15-bis(4-boronophenyl)-porphyrin; PA—Photoacoustic; ROS—Reactive oxygen species; TP-Por—Triphenylene-porphyrin; BSA—Bovine serum albumin; SHNPs—Semiconductor heterojunction nanoparticles; RT—Radiotherapy; CT—Computed tomography; TAA—Thioacetamide
图 7 BiOI/BiOIO3纳米复合材料[94]体内电子计算机断层扫描(CT)成像图 (a)、肿瘤治疗效果 ((b)~(d))、抗肿瘤机制示意图 (e)；CeVO4/Au NCs[131]制备与近红外(NIR)光介导的PTT和PDT肿瘤成像与治疗示意图 (f)、TEM图像 (g)、HR-TEM图像(h) 、EDS元素图 (i)
Figure 7. In vivo computed tomography (CT) imaging (a) , the graph of tumor treatment effects ((b)-(d)) and schematic representation of the antitumor mechanism of BiOI/BiOIO3 nanocomposite (e)[94]; lmatic representation of the preparation and near-infrared (NIR) light-mediated photothermal-photodynamic combined imaging and treatment of tumors (f) , TEM image (g) , HR-TEM image (h) and EDS elemental diagrams (i) of CeVO4/Au NCs[131]
图 8 多模态诊疗一体的应用与机制 (a)[127]；Bi-Bi2S3/BSA&FA NPs[124]应用于多模态成像(CT/PA)引导的肿瘤光热治疗机制示意图 (b)、促进CT成像的效果 (c)、成像引导的光热疗法效果 (d)；CSA NPs[127]靶向效果(e)、促进CT成像的效果 ((f)~(g))；用于多模态成像的放射-光热协同肿瘤治疗机制示意图 (h)
Figure 8. Application and mechanism of multimodal therapy in one (a)[127]; schematic diagram of the mechanism of radiation-photothermal therapy applied to multimodal imaging (CT/PA)-guided tumor therapy (b) , effect of promoting CT imaging (c) and the effect of imaging-guided photothermal therapy (d) of Bi-Bi2S3/BSA&FA NPs[124]; figures of targeting effect (e) , effect of promoting CT imaging ((f)-(g)) and schematic diagram of the mechanism of radiation-photothermal synergistic tumor therapy applied to multimodal imaging (h) of CSA NPs[127]
表 1 不同异质结材料在肿瘤诊疗一体化领域的研究
Table 1. Study of different heterojunction materials in the integration of tumor diagnosis and treatment
Heterojunction Treatment method Imaging methods Time Ref BiOI-Bi2S3 RT/PDT/PTT CT/PA 2017 [94] Bi2S3-Au PTT CT 2017 [121] AuNC/Fe(OH)3 PTT CT/MRI 2018 [122] NPs(Ag2S, Ag2Se, UCNP)@ZIF-8@Au Chemo/PTT CT/FL/PA 2018 [123] Bi−Bi2S3 PTT CT/PA 2019 [124] Bi2Se3/MoSe2/Bi2Se3 Chemo/PDT/PTT CT/PT 2019 [125] CeVO4/Ag PDT/PTT PA 2019 [126] Cu2−xSe/Au RT/PTT CT/PA/SPECT 2019 [127] Fe3O4−Ag2S PTT CT/MRI 2019 [128] MoSe2/Bi2Se3 Chemo/PDT/PTT CT/PT 2019 [125] NdVO4/Au PDT PA/PT 2019 [129] UCNPs@Pd PTT MRI/UCL 2019 [130] CeVO4/Au PDT/PTT PA/PT 2020 [131] Co3S4@N-doped carbon Chemo PDT/PTT MRI/PT 2020 [132] FeTiO3@Fe2O3 CDT/PDT/PTT FL/PT 2020 [133] Fe2O3-FeS2 CDT/PDT/PTT PA/PT 2020 [101] Se/Au/Fe−EpC RT CT/MRI/PA 2020 [134] Notes: PA—Photoacoustce; MRI—Magnetic resonance imaging; FL—Fluorescence; SPECT—Single photon emission computed tomography; UCL—Up-conversion luminescence. 
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