<i>In vivo</i> tumor imaging and therapy based on near-infrared cadmium-free quantum dots_Journal of Biomedical Engineering

Authors：

LI Xiaoqi ¹ , SUN Xiao ¹ , LIN Hua ² , ZHANG Peisen ¹ ,  JIAO Mingxia ¹ ,  ZHANG Ni ²

1. College of Chemical and Molecular Engineering, Qingdao University of Science and Technology, Qingdao, Shandong 266042, P. R. China;
2. West China Hospital of Sichuan University, Chengdu 610041, P. R. China;

Corresponding author：

Keywords：

Quantum dots; Near-infrared photoluminescence; In vivo imaging; Tumor therapy

DOI：

10.7507/1001-5515.202404002

Video：

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Near-infrared fluorescence imaging technology, which possesses superior advantages including real-time and fast imaging, high spatial and temporal resolution, and deep tissue penetration, shows great potential for tumor imaging in vivo and therapy. Ⅰ-Ⅲ-Ⅵ quantum dots exhibit high brightness, broad excitation, easily tunable emission wavelength and superior stability, and do not contain highly toxic heavy metal elements such as cadmium or lead. These advantages make Ⅰ-Ⅲ-Ⅵ quantum dots attract widespread attention in biomedical field. This review summarizes the recent advances in the controlled synthesis of Ⅰ-Ⅲ-Ⅵ quantum dots and their applications in tumor imaging in vivo and therapy. Firstly, the organic-phase and aqueous-phase synthesis of Ⅰ-Ⅲ-Ⅵ quantum dots as well as the strategies for regulating the near-infrared photoluminescence are briefly introduced; secondly, representative biomedical applications of near-infrared-emitting cadmium-free quantum dots including early diagnosis of tumor, lymphatic imaging, drug delivery, photothermal and photodynamic therapy are emphatically discussed; lastly, perspectives on the future directions of developing quantum dots for biomedical application and the faced challenges are discussed. This paper may provide guidance and reference for further research and clinical translation of cadmium-free quantum dots in tumor diagnosis and treatment.

Citation： LI Xiaoqi, SUN Xiao, LIN Hua, ZHANG Peisen, JIAO Mingxia, ZHANG Ni. In vivo tumor imaging and therapy based on near-infrared cadmium-free quantum dots. Journal of Biomedical Engineering, 2024, 41(3): 620-626. doi: 10.7507/1001-5515.202404002 Copy

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4.	Yang H, Li R, Zhang Y, et al. Colloidal alloyed quantum dots with enhanced photoluminescence quantum yield in the NIR-Ⅱ window. J Am Chem Soc, 2021, 143(6): 2601-2607.
5.	林倩黎, 叶远馨, 李美, 等. 量子点在检验医学领域中的研究进展. 华西医学, 2021, 36(8): 1001-1006.
6.	Jung B K, Yoo H, Seo B, et al. High-affinity ligand-enhanced passivation of group Ⅲ-V colloidal quantum dots for sensitive near-infrared photodetection. ACS Energy Lett, 2024, 9(2): 504-512.
7.	Jiang Y, Zhao T, Xu W, et al. Red/NIR C-dots: a perspective from carbon precursors, photoluminescence tuning and bioapplications. Carbon, 2024, 219: 118838.
8.	Lim L J, Zhao X, Tan Z. Non-toxic CuInS₂/ZnS colloidal quantum dots for near-infrared light-emitting diodes. Adv Mater, 2023, 35(28): e2301887.
9.	Li S, Jung S, Chung W, et al. Defect engineering of ternary Cu-In-Se quantum dots for boosting photoelectrochemical hydrogen generation. Carbon Energy, 2023, 5(12): e384.
10.	Hasanirokh K, Asgari A, Mohammadi S. Fabrication of a light-emitting device based on the CdS/ZnS spherical quantum dots. J Eur Opt Soc-Rapid, 2021, 17(1): 26.
11.	孙静文, 魏国光, 钱余义, 等. 硫化铅量子点的结肠癌近红外IIb区荧光成像研究. 药学学报, 2020, 55(7): 1699-1706.
12.	房诗玉, 刘振宇, 金佳杰, 等. 碲镉汞量子点的离子交换能带调控及其近红外自吸收性质. 红外与毫米波学报, 2022, 41(2): 377-383.
13.	Li Y, Zhang P, Tang W, et al. Bright, magnetic NIR-Ⅱ quantum dot probe for sensitive dual-modality imaging and intensive combination therapy of cancer. ACS Nano, 2022, 16(5): 8076-8094.
14.	Liu H, Cai P, McHugh K J, et al. Aqueous synthesis of bright near-infrared-emitting Zn-Cu-In-Se quantum dots for multiplexed detection of tumor markers. Nano Res, 2022, 15(9): 8351-8359.
15.	Yang L, Zhang S, Xu B, et al. I-Ⅲ-Ⅵ quantum dots and derivatives: design, synthesis, and properties for light-emitting diodes. Nano Lett, 2023, 23(7): 2443-2453.
16.	Lu H, Hu Z, Zhou W, et al. Synthesis and structure design of I-Ⅲ-Ⅵ quantum dots for white light-emitting diodes. Mater Chem Front, 2022, 6(4): 418-429.
17.	Zhang X, Wang T, Lin Q, et al. Highly efficient near-infrared light-emitting diodes based on Zn: CuInSe₂/ZnS//ZnS quantum dots with double shell engineering. Opt Express, 2022, 30(16): 29449-29460.
18.	McHugh K J, Jing L, Severt S Y, et al. Biocompatible near-infrared quantum dots delivered to the skin by microneedle patches record vaccination. Sci Transl Med, 2019, 11(523): eaay7162.
19.	Langevin M A, Ritcey A M, Allen C N. Air-stable near-infrared AgInSe₂ nanocrystals. ACS Nano, 2014, 8(4): 3476-3482.
20.	Ning J, Xiong Y, Huang F, et al. Growth of multinary copper-based sulfide shells on CuInSe₂ nanocrystals for significant improvement of their near-infrared emission. Chem Mater, 2020, 32(18): 7842-7849.
21.	廉纬, 方泽铠, 涂大涛, 等. 模板法控制合成AgInSe₂: Zn²⁺近红外荧光量子点及其生物标记应用. 化学学报, 2022, 80(5): 625-632.
22.	Qu S, Yuan X, Li Y, et al. Aqueous synthesis of composition-tuned defects in CuInSe₂ nanocrystals for enhanced visible-light photocatalytic H₂ evolution. Nanoscale Adv, 2021, 3(8): 2334-2342.
23.	Yang X, Li Y, Zhang P, et al. Building in biologically appropriate multifunctionality in aqueous copper indium selenide-based quantum dots. Nanoscale, 2023, 15(33): 13603-13616.
24.	Jiao M, Portniagin A S, Luo X, et al. Semiconductor nanocrystals emitting in the second near-infrared window: optical properties and application in biomedical imaging. Adv Opt Mater, 2022, 10(14): 2200226.
25.	Yang G, Xia J, Dai X, et al. A targeted multi-crystalline manganese oxide as a tumor-selective nano-sized MRI contrast agent for early and accurate diagnosis of tumors. Int J Nanomed, 2024, 19: 527-540.
26.	Li W, Liu J B, Hou L K, et al. Liquid biopsy in lung cancer: significance in diagnostics, prediction, and treatment monitoring. Mol Cancer, 2022, 21(1): 25.
27.	de Souza N, Zhao S, Bodenmiller B. Multiplex protein imaging in tumour biology. Nat Rev Cancer, 2024, 24(13): 171-191.
28.	Lian W, Tu D, Hu P, et al. Broadband excitable NIR-II luminescent nano-bioprobes based on CuInSe₂ quantum dots for the detection of circulating tumor cells. Nano Today, 2020, 35: 100943.
29.	Lee J Y, Heon Nam D, Oh M H, et al. Serum-stable quantum dot--protein hybrid nanocapsules for optical bio-imaging. Nanotechnology, 2014, 25(17): 175702.
30.	Miao D, Shi J, Lv Q, et al. NAT10-mediated ac⁴C-modified ANKZF1 promotes tumor progression and lymphangiogenesis in clear-cell renal cell carcinoma by attenuating YWHAE-driven cytoplasmic retention of YAP1. Cancer Commun, 2024, 44(3): 361-383.
31.	Zhou X, Fan Y, Li S, et al. Molecular engineering of bright NIR-I/NIR-II nanofluorophores for high-resolution bioimaging and tumor detection in vivo. Nano Lett, 2024, 24(5): 1792-1800.
32.	Meng X, Li H, Chen Y, et al. In vivo precision evaluation of lymphatic function by SWIR luminescence imaging with PbS quantum dots. Adv Sci, 2023, 10(7): e2206579.
33.	Pons T, Pic E, Lequeux N, et al. Cadmium-free CuInS₂/ZnS quantum dots for sentinel lymph node imaging with reduced toxicity. ACS Nano, 2010, 4(5): 2531-2538.
34.	Sun X, Shi M, Zhang C, et al. Fluorescent Ag-In-S/ZnS quantum dots for tumor drainage lymph node imaging in vivo. ACS Appl Nano Mater, 2021, 4(2): 1029-1037.
35.	Boas D, van Teijlingen A, Shpilt Z, et al. A multifunctional drug delivery system based on switchable peptide-stabilized emulsions. Chem, 2024. DOI: 10.1016/j.chempr.2024.02.003.
36.	Wu J, Ma T, Zhu M, et al. A pluripotential neutrophil-mimic nanovehicle modulates immune microenvironment with targeted drug delivery for augmented antitumor chemotherapy. ACS Nano, 2024, 18(7): 5864-5877.
37.	Yan J, Yu H, Liu C, et al. Low-temperature photothermal-chemotherapy enhancing tumor immunotherapy by tetrahedral framework nucleic acids nanogels based drug delivery system. Chem Eng J, 2024, 481: 148616.
38.	Li Z, Xu K, Qin L, et al. Hollow nanomaterials in advanced drug delivery systems: from single-to multiple shells. Adv Mater, 2023, 35(12): e2203890.
39.	Wu P, Ou K, Chen J, et al. Methotrexate-conjugated AgInS₂/ZnS quantum dots for optical imaging and drug delivery. Mater Lett, 2014, 128: 412-416.
40.	Akbarzadeh M, Babaei M, Abnous K, et al. Hybrid silica-coated Gd-Zn-Cu-In-S/ZnS bimodal quantum dots as an epithelial cell adhesion molecule targeted drug delivery and imaging system. Int J Pharm, 2019, 570: 118645.
41.	Tang Y, Bisoyi H K, Chen X M, et al. Pyroptosis-mediated synergistic photodynamic and photothermal immunotherapy enabled by a tumor-membrane-targeted photosensitive dimer. Adv Mater, 2023, 35(25): e2300232.
42.	Li S, Xu B, Lu M, et al. Tensile-strained palladium nanosheets for synthetic catalytic therapy and phototherapy. Adv Mater, 2022, 34(32): e2202609.
43.	Zhang Z, Kang M, Tan H, et al. The fast-growing field of photo-driven theranostics based on aggregation-induced emission. Chem Soc Rev, 2022, 51(6): 1983-2030.
44.	Mayerhoefer M E, Raderer M, Lamm W, et al. CXCR4 PET/MRI for follow-up of gastric mucosa-associated lymphoid tissue lymphoma after first-line helicobacter pylori eradication. Blood, 2022, 139(2): 240-244.
45.	Lv G, Guo W, Zhang W, et al. Near-infrared emission CuInS/ZnS quantum dots: all-in-one theranostic nanomedicines with intrinsic fluorescence/photoacoustic imaging for tumor phototherapy. ACS Nano, 2016, 10(10): 9637-9645.

1. Moghaddam F D, Zare E N, Hassanpour M, et al. Chitosan-based nanosystems for cancer diagnosis and therapy: stimuli-responsive, immune response, and clinical studies. Carbohyd Polym, 2024, 330: 121839.
2. 徐睿锋, 孙鑫, 田雨, 等. 《2016年中国癌症发病死亡数据》要点解读. 中国胸心血管外科临床杂志, 2024, 31(3): 343-356.
3. Skripka A, Mendez-Gonzalez D, Marin R, et al. Near infrared bioimaging and biosensing with semiconductor and rare-earth nanoparticles: recent developments in multifunctional nanomaterials. Nanoscale Adv, 2021, 3(22): 6310-6329.
4. Yang H, Li R, Zhang Y, et al. Colloidal alloyed quantum dots with enhanced photoluminescence quantum yield in the NIR-Ⅱ window. J Am Chem Soc, 2021, 143(6): 2601-2607.
5. 林倩黎, 叶远馨, 李美, 等. 量子点在检验医学领域中的研究进展. 华西医学, 2021, 36(8): 1001-1006.
6. Jung B K, Yoo H, Seo B, et al. High-affinity ligand-enhanced passivation of group Ⅲ-V colloidal quantum dots for sensitive near-infrared photodetection. ACS Energy Lett, 2024, 9(2): 504-512.
7. Jiang Y, Zhao T, Xu W, et al. Red/NIR C-dots: a perspective from carbon precursors, photoluminescence tuning and bioapplications. Carbon, 2024, 219: 118838.
8. Lim L J, Zhao X, Tan Z. Non-toxic CuInS₂/ZnS colloidal quantum dots for near-infrared light-emitting diodes. Adv Mater, 2023, 35(28): e2301887.
9. Li S, Jung S, Chung W, et al. Defect engineering of ternary Cu-In-Se quantum dots for boosting photoelectrochemical hydrogen generation. Carbon Energy, 2023, 5(12): e384.
10. Hasanirokh K, Asgari A, Mohammadi S. Fabrication of a light-emitting device based on the CdS/ZnS spherical quantum dots. J Eur Opt Soc-Rapid, 2021, 17(1): 26.
11. 孙静文, 魏国光, 钱余义, 等. 硫化铅量子点的结肠癌近红外IIb区荧光成像研究. 药学学报, 2020, 55(7): 1699-1706.
12. 房诗玉, 刘振宇, 金佳杰, 等. 碲镉汞量子点的离子交换能带调控及其近红外自吸收性质. 红外与毫米波学报, 2022, 41(2): 377-383.
13. Li Y, Zhang P, Tang W, et al. Bright, magnetic NIR-Ⅱ quantum dot probe for sensitive dual-modality imaging and intensive combination therapy of cancer. ACS Nano, 2022, 16(5): 8076-8094.
14. Liu H, Cai P, McHugh K J, et al. Aqueous synthesis of bright near-infrared-emitting Zn-Cu-In-Se quantum dots for multiplexed detection of tumor markers. Nano Res, 2022, 15(9): 8351-8359.
15. Yang L, Zhang S, Xu B, et al. I-Ⅲ-Ⅵ quantum dots and derivatives: design, synthesis, and properties for light-emitting diodes. Nano Lett, 2023, 23(7): 2443-2453.
16. Lu H, Hu Z, Zhou W, et al. Synthesis and structure design of I-Ⅲ-Ⅵ quantum dots for white light-emitting diodes. Mater Chem Front, 2022, 6(4): 418-429.
17. Zhang X, Wang T, Lin Q, et al. Highly efficient near-infrared light-emitting diodes based on Zn: CuInSe₂/ZnS//ZnS quantum dots with double shell engineering. Opt Express, 2022, 30(16): 29449-29460.
18. McHugh K J, Jing L, Severt S Y, et al. Biocompatible near-infrared quantum dots delivered to the skin by microneedle patches record vaccination. Sci Transl Med, 2019, 11(523): eaay7162.
19. Langevin M A, Ritcey A M, Allen C N. Air-stable near-infrared AgInSe₂ nanocrystals. ACS Nano, 2014, 8(4): 3476-3482.
20. Ning J, Xiong Y, Huang F, et al. Growth of multinary copper-based sulfide shells on CuInSe₂ nanocrystals for significant improvement of their near-infrared emission. Chem Mater, 2020, 32(18): 7842-7849.
21. 廉纬, 方泽铠, 涂大涛, 等. 模板法控制合成AgInSe₂: Zn²⁺近红外荧光量子点及其生物标记应用. 化学学报, 2022, 80(5): 625-632.
22. Qu S, Yuan X, Li Y, et al. Aqueous synthesis of composition-tuned defects in CuInSe₂ nanocrystals for enhanced visible-light photocatalytic H₂ evolution. Nanoscale Adv, 2021, 3(8): 2334-2342.
23. Yang X, Li Y, Zhang P, et al. Building in biologically appropriate multifunctionality in aqueous copper indium selenide-based quantum dots. Nanoscale, 2023, 15(33): 13603-13616.
24. Jiao M, Portniagin A S, Luo X, et al. Semiconductor nanocrystals emitting in the second near-infrared window: optical properties and application in biomedical imaging. Adv Opt Mater, 2022, 10(14): 2200226.
25. Yang G, Xia J, Dai X, et al. A targeted multi-crystalline manganese oxide as a tumor-selective nano-sized MRI contrast agent for early and accurate diagnosis of tumors. Int J Nanomed, 2024, 19: 527-540.
26. Li W, Liu J B, Hou L K, et al. Liquid biopsy in lung cancer: significance in diagnostics, prediction, and treatment monitoring. Mol Cancer, 2022, 21(1): 25.
27. de Souza N, Zhao S, Bodenmiller B. Multiplex protein imaging in tumour biology. Nat Rev Cancer, 2024, 24(13): 171-191.
28. Lian W, Tu D, Hu P, et al. Broadband excitable NIR-II luminescent nano-bioprobes based on CuInSe₂ quantum dots for the detection of circulating tumor cells. Nano Today, 2020, 35: 100943.
29. Lee J Y, Heon Nam D, Oh M H, et al. Serum-stable quantum dot--protein hybrid nanocapsules for optical bio-imaging. Nanotechnology, 2014, 25(17): 175702.
30. Miao D, Shi J, Lv Q, et al. NAT10-mediated ac⁴C-modified ANKZF1 promotes tumor progression and lymphangiogenesis in clear-cell renal cell carcinoma by attenuating YWHAE-driven cytoplasmic retention of YAP1. Cancer Commun, 2024, 44(3): 361-383.
31. Zhou X, Fan Y, Li S, et al. Molecular engineering of bright NIR-I/NIR-II nanofluorophores for high-resolution bioimaging and tumor detection in vivo. Nano Lett, 2024, 24(5): 1792-1800.
32. Meng X, Li H, Chen Y, et al. In vivo precision evaluation of lymphatic function by SWIR luminescence imaging with PbS quantum dots. Adv Sci, 2023, 10(7): e2206579.
33. Pons T, Pic E, Lequeux N, et al. Cadmium-free CuInS₂/ZnS quantum dots for sentinel lymph node imaging with reduced toxicity. ACS Nano, 2010, 4(5): 2531-2538.
34. Sun X, Shi M, Zhang C, et al. Fluorescent Ag-In-S/ZnS quantum dots for tumor drainage lymph node imaging in vivo. ACS Appl Nano Mater, 2021, 4(2): 1029-1037.
35. Boas D, van Teijlingen A, Shpilt Z, et al. A multifunctional drug delivery system based on switchable peptide-stabilized emulsions. Chem, 2024. DOI: 10.1016/j.chempr.2024.02.003.
36. Wu J, Ma T, Zhu M, et al. A pluripotential neutrophil-mimic nanovehicle modulates immune microenvironment with targeted drug delivery for augmented antitumor chemotherapy. ACS Nano, 2024, 18(7): 5864-5877.
37. Yan J, Yu H, Liu C, et al. Low-temperature photothermal-chemotherapy enhancing tumor immunotherapy by tetrahedral framework nucleic acids nanogels based drug delivery system. Chem Eng J, 2024, 481: 148616.
38. Li Z, Xu K, Qin L, et al. Hollow nanomaterials in advanced drug delivery systems: from single-to multiple shells. Adv Mater, 2023, 35(12): e2203890.
39. Wu P, Ou K, Chen J, et al. Methotrexate-conjugated AgInS₂/ZnS quantum dots for optical imaging and drug delivery. Mater Lett, 2014, 128: 412-416.
40. Akbarzadeh M, Babaei M, Abnous K, et al. Hybrid silica-coated Gd-Zn-Cu-In-S/ZnS bimodal quantum dots as an epithelial cell adhesion molecule targeted drug delivery and imaging system. Int J Pharm, 2019, 570: 118645.
41. Tang Y, Bisoyi H K, Chen X M, et al. Pyroptosis-mediated synergistic photodynamic and photothermal immunotherapy enabled by a tumor-membrane-targeted photosensitive dimer. Adv Mater, 2023, 35(25): e2300232.
42. Li S, Xu B, Lu M, et al. Tensile-strained palladium nanosheets for synthetic catalytic therapy and phototherapy. Adv Mater, 2022, 34(32): e2202609.
43. Zhang Z, Kang M, Tan H, et al. The fast-growing field of photo-driven theranostics based on aggregation-induced emission. Chem Soc Rev, 2022, 51(6): 1983-2030.
44. Mayerhoefer M E, Raderer M, Lamm W, et al. CXCR4 PET/MRI for follow-up of gastric mucosa-associated lymphoid tissue lymphoma after first-line helicobacter pylori eradication. Blood, 2022, 139(2): 240-244.
45. Lv G, Guo W, Zhang W, et al. Near-infrared emission CuInS/ZnS quantum dots: all-in-one theranostic nanomedicines with intrinsic fluorescence/photoacoustic imaging for tumor phototherapy. ACS Nano, 2016, 10(10): 9637-9645.

Journal of Biomedical Engineering

In vivo tumor imaging and therapy based on near-infrared cadmium-free quantum dots

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