Iron–silver-modified quantum dots act as efficient catalysts in anti-cancer multitherapy through controlled, ultrasound-induced oxidation
Source abstract
Abstract
Chemodynamic therapy and sonodynamic therapy are two promising tumour therapeutic strategies. However, lack of highly effective sonosensitizers and control over chemodynamic therapy limit their application. Here we synthesize silver-doped zinc selenide quantum dots with atomically dispersed superficial Fe and show that they act as efficient sonosensitizers, catalysers and immunoreagents. Surface modification with an in situ self-assembly peptide drives accumulation in tumours. Superficial FeIII remains stable and converts to FeII only under ultrasonic processing, reverting to FeIII upon ultrasound cessation. Under ultrasound stimulation, superficial Fe undergoes valence change with concomitant amelioration of the hypoxic tumour microenvironment and production of sonodynamic therapy-beneficial hydroxyl radicals. Furthermore, silver doping suppressed nonradiative recombination of excitons, leading to improved production of singlet oxygen. Meanwhile, selenium promotes robust systemic immune responses for the inhibition of tumour metastases. This nano-platform allows control of valence switching of atomically dispersed catalysts, representing an effective tool for chemodynamic/sonodynamic/immunotherapy.
Source: europepmc · Quality: candidate unverified · Source record ↗
Research context
OpenAlex topics: Advanced Nanomaterials in Catalysis · Nanoplatforms for cancer theranostics · Advanced Photocatalysis Techniques
SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.
References (32)
Show source-provided references
1. Chen, R. et al. Photoacoustic molecular imaging-escorted adipose photodynamic–browning synergy for fighting obesity with virus-like complexes. Nat. Nanotechnol. 16, 455–465 (2021).10.1038/s41565-020-00844-6 ↗
2. Wang, D. et al. Sub-nanosheet induced inverse growth of negative valency Au clusters for tumor treatment by enhanced oxidative stress. Angew. Chem. Int. Ed. 63, e202410649 (2024).10.1002/anie.202410649 ↗
3. Fan, Y., Liu, S., Yi, Y., Rong, H. & Zhang, J. Catalytic nanomaterials toward atomic levels for biomedical applications: from metal clusters to single-atom catalysts. ACS Nano 15, 2005–2037 (2021).10.1021/acsnano.0c06962 ↗
4. Fan, K. et al. In vivo guiding nitrogen-doped carbon nanozyme for tumor catalytic therapy. Nat. Commun. 9, 1440 (2018).10.1038/s41467-018-03903-8 ↗
5. Li, J., Stephanopoulos, M. F. & Xia, Y. Introduction: heterogeneous single-atom catalysis. Chem. Rev. 120, 11699–11702 (2020).10.1021/acs.chemrev.0c01097 ↗
6. Ji, S. et al. Matching the kinetics of natural enzymes with a single-atom iron nanozyme. Nat. Catal. 4, 407–417 (2021).10.1038/s41929-021-00609-x ↗
7. Yin, Y. et al. Boosting Fenton-like reactions via single atom Fe catalysis. Environ. Sci. Technol. 53, 11391–11400 (2019).10.1021/acs.est.9b03342 ↗
8. Qian, X., Zhang, J., Gu, Z. & Chen, Y. Nanocatalysts-augmented Fenton chemical reaction for nanocatalytic tumor therapy. Biomaterials 211, 1–13 (2019).10.1016/j.biomaterials.2019.04.023 ↗
9. Yu, B., Wang, W., Sun, W., Jiang, C. & Lu, L. Defect engineering enables synergistic action of enzyme-mimicking active centers for high-efficiency tumor therapy. J. Am. Chem. Soc. 143, 8855–8865 (2021).10.1021/jacs.1c03510 ↗
10. Qin, X. et al. Peroxisome inspired hybrid enzyme nanogels for chemodynamic and photodynamic therapy. Nat. Commun. 12, 5243 (2021).10.1038/s41467-021-25561-z ↗
11. Huang, P. et al. Metalloporphyrin-encapsulated biodegradable nanosystems for highly efficient magnetic resonance imaging-guided sonodynamic cancer therapy. J. Am. Chem. Soc. 139, 1275–1284 (2017).10.1021/jacs.6b11846 ↗
12. Wang, D. et al. Precise magnetic resonance imaging-guided sonodynamic therapy for drug-resistant bacterial deep infection. Biomaterials 264, 120386 (2021).10.1016/j.biomaterials.2020.120386 ↗
13. Wang, D., Zhu, Y., Wan, X., Zhang, X. & Zhang, J. Colloidal semiconductor nanocrystals for biological photodynamic therapy applications: recent progress and perspectives. Prog. Nat. Sci. Mater. Int. 30, 443–455 (2020).10.1016/j.pnsc.2020.08.016 ↗
14. Linterman, M. A. & Denton, A. E. Selenium saves ferroptotic TFH cells to fortify the germinal center. Nat. Immunol. 22, 1074–1076 (2021).10.1038/s41590-021-01007-y ↗
15. Gao, S. et al. Selenium-containing nanoparticles combine the NK cells mediated immunotherapy with radiotherapy and chemotherapy. Adv. Mater. 32, 1907568 (2020).10.1002/adma.201907568 ↗
16. Feng, Z., Wang, H., Chen, X. & Xu, B. Self-assembling ability determines the activity of enzyme-instructed self-assembly for inhibiting cancer cells. J. Am. Chem. Soc. 139, 15377–15384 (2017).10.1021/jacs.7b07147 ↗
17. Zhang, L. et al. Transformable peptide nanoparticles arrest HER2 signalling and cause cancer cell death in vivo. Nat. Nanotechnol. 15, 145–153 (2020).10.1038/s41565-019-0626-4 ↗
18. Gui, J. et al. Phosphine-initiated cation exchange for precisely tailoring composition and properties of semiconductor nanostructures: old concept, new applications. Angew. Chem. Int. Ed. 127, 3754–3758 (2015).10.1002/ange.201410053 ↗
19. Di, Q. et al. High-performance quantum dots with synergistic doping and oxide shell protection synthesized by cation exchange conversion of ternary-composition nanoparticles. J. Phys. Chem. Lett. 10, 2606–2615 (2019).10.1021/acs.jpclett.9b00617 ↗
20. Jing, X. et al. Role of hypoxia in cancer therapy by regulating the tumor microenvironment. Mol. Cancer 18, 157 (2019).10.1186/s12943-019-1089-9 ↗
21. Wu, C. et al. Biodegradable Fe(III)@WS2-PVP nanocapsules for redox reaction and TME-enhanced nanocatalytic, photothermal, and chemotherapy. Adv. Funct. Mater. 29, 1901722 (2019).10.1002/adfm.201901722 ↗
22. Huang, L., Chen, J., Gan, L., Wang, J. & Dong, S. Single-atom nanozymes. Sci. Adv. 5, eaav5490 (2019).10.1126/sciadv.aav5490 ↗
23. Ma, W. et al. A single-atom Fe–N4 catalytic site mimicking bifunctional antioxidative enzymes for oxidative stress cytoprotection. Chem. Commun. 55, 159–162 (2019).10.1039/C8CC08116F ↗
24. Bai, J., Jia, X., Zhen, W., Cheng, W. & Jiang, X. A facile ion-doping strategy to regulate tumor microenvironments for enhanced multimodal tumor theranostics. J. Am. Chem. Soc. 140, 106–109 (2018).10.1021/jacs.7b11114 ↗
25. Cheng, D.-B. et al. Autocatalytic morphology transformation platform for targeted drug accumulation. J. Am. Chem. Soc. 141, 4406–4411 (2019).10.1021/jacs.8b13512 ↗
26. Li, G. et al. Fluorescence and optical activity of chiral CdTe quantum dots in their interaction with amino acids. ACS Nano 14, 4196–4205 (2020).10.1021/acsnano.9b09101 ↗
27. Branca, C. et al. Role of the OH and NH vibrational groups in polysaccharide-nanocomposite interactions: A FTIR-ATR study on chitosan and chitosan/clay films. Polymer 99, 614–622 (2016).10.1016/j.polymer.2016.07.086 ↗
28. Pillai, C., Paul, W. & Sharma, C. P. Chitin and chitosan polymers: chemistry, solubility and fiber formation. Prog. Polym. Sci. 34, 641–678 (2009).10.1016/j.progpolymsci.2009.04.001 ↗
29. Liu, F.-H. et al. Near-infrared laser-driven in situ self-assembly as a general strategy for deep tumor therapy. Nano Lett. 18, 6577–6584 (2018).10.1021/acs.nanolett.8b03174 ↗
30. Song, X., Feng, L., Liang, C., Yang, K. & Liu, Z. Ultrasound triggered tumor oxygenation with oxygen-shuttle nanoperfluorocarbon to overcome hypoxia-associated resistance in cancer therapies. Nano Lett. 16, 6145–6153 (2016).10.1021/acs.nanolett.6b02365 ↗
31. Meng, Z. et al. Light-triggered in situ gelation to enable robust photodynamic-immunotherapy by repeated stimulations. Adv. Mater. 31, 1900927 (2019).10.1002/adma.201900927 ↗
32. Shao, Y. et al. Engineering of upconverted metal–organic frameworks for near-infrared light-triggered combinational photodynamic/chemo-/immunotherapy against hypoxic tumors. J. Am. Chem. Soc. 142, 3939–3946 (2020).10.1021/jacs.9b12788 ↗