Triplet Electron Exchange in Carbon Nanodots‐assisted Long‐persistent near‐infrared Chemiluminescence for Oncology Synergistic Imaging and Therapy

Abstract In classical photodynamic therapy, tumor cells are killed by the cytotoxic species via type‐I/II photochemical reactions, seriously limited by the external photoexcitation and hypoxia. Herein, the electron transfer mechanism between fluorophores and peroxalate‐H2O2 reaction is investigated...

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Main Authors: Run‐Wei Song, Tian‐Ci Jiang, Xue‐Yang Zhang, Cheng‐Long Shen, Qing Lou, Chong‐Xin Shan
Format: Article
Language:English
Published: Wiley 2025-02-01
Series:Advanced Science
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Online Access:https://doi.org/10.1002/advs.202411898
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author Run‐Wei Song
Tian‐Ci Jiang
Xue‐Yang Zhang
Cheng‐Long Shen
Qing Lou
Chong‐Xin Shan
author_facet Run‐Wei Song
Tian‐Ci Jiang
Xue‐Yang Zhang
Cheng‐Long Shen
Qing Lou
Chong‐Xin Shan
author_sort Run‐Wei Song
collection DOAJ
description Abstract In classical photodynamic therapy, tumor cells are killed by the cytotoxic species via type‐I/II photochemical reactions, seriously limited by the external photoexcitation and hypoxia. Herein, the electron transfer mechanism between fluorophores and peroxalate‐H2O2 reaction is investigated and the singlet/triplet electron exchange is utilized to achieve long‐persistent chemiluminescence imaging and synergistic type‐I/II/III photodynamic therapy. As a proof‐of‐concept, the photosensitizers of carbon nanodots (CDs)‐loaded chlorin e6 (CDs‐Ce6) are designed and integrated with the peroxalate molecules, and the as‐prepare polymer carbon nanodots (p‐CDs) exhibit novel tumor microenvironment (TME)‐responsive long‐persistent near‐infrared CL and photochemical reactions, evoking the in vivo imaging and synergistic dynamic therapy in tumor tissue. Mechanistically, the excess reactive oxygen species in TME can trigger the chemically initiated singlet/triplet electron exchange between the hydrophobic CDs‐Ce6 and peroxalate‐derived 1,2‐dioxetanes and thus the excess excited singlet/triplet electron of the CDs‐Ce6 can ensure the long‐persistent near‐infrared CL, type I/II photochemical production of hydroxyl radicals, superoxide radical and singlet oxygen, and type III photochemical damage of maladjusted biomacromolecules, enabling the long‐persistent near‐infrared biological imaging and enhanced cancer therapy. These results shed a new sight into the energy transfer mechanism in chemiluminescence and pave a new sight into the architecture of multifunctional theragnostic nanoplatforms.
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spelling doaj-art-93761e7b2bb0430385f7335b02daefe72025-02-04T13:14:54ZengWileyAdvanced Science2198-38442025-02-01125n/an/a10.1002/advs.202411898Triplet Electron Exchange in Carbon Nanodots‐assisted Long‐persistent near‐infrared Chemiluminescence for Oncology Synergistic Imaging and TherapyRun‐Wei Song0Tian‐Ci Jiang1Xue‐Yang Zhang2Cheng‐Long Shen3Qing Lou4Chong‐Xin Shan5Henan Key Laboratory of Diamond Optoelectronic Materials and Devices Key Laboratory of Material Physics Ministry of Education and School of Physics and Laboratory of Zhongyuan Light Zhengzhou University Zhengzhou 450052 ChinaDepartment of Respiratory and Critical Care Medicine The First Affiliated Hospital of Zhengzhou University Zhengzhou 450052 ChinaCollege of Public Health Zhengzhou University Zhengzhou 450052 ChinaHenan Key Laboratory of Diamond Optoelectronic Materials and Devices Key Laboratory of Material Physics Ministry of Education and School of Physics and Laboratory of Zhongyuan Light Zhengzhou University Zhengzhou 450052 ChinaHenan Key Laboratory of Diamond Optoelectronic Materials and Devices Key Laboratory of Material Physics Ministry of Education and School of Physics and Laboratory of Zhongyuan Light Zhengzhou University Zhengzhou 450052 ChinaHenan Key Laboratory of Diamond Optoelectronic Materials and Devices Key Laboratory of Material Physics Ministry of Education and School of Physics and Laboratory of Zhongyuan Light Zhengzhou University Zhengzhou 450052 ChinaAbstract In classical photodynamic therapy, tumor cells are killed by the cytotoxic species via type‐I/II photochemical reactions, seriously limited by the external photoexcitation and hypoxia. Herein, the electron transfer mechanism between fluorophores and peroxalate‐H2O2 reaction is investigated and the singlet/triplet electron exchange is utilized to achieve long‐persistent chemiluminescence imaging and synergistic type‐I/II/III photodynamic therapy. As a proof‐of‐concept, the photosensitizers of carbon nanodots (CDs)‐loaded chlorin e6 (CDs‐Ce6) are designed and integrated with the peroxalate molecules, and the as‐prepare polymer carbon nanodots (p‐CDs) exhibit novel tumor microenvironment (TME)‐responsive long‐persistent near‐infrared CL and photochemical reactions, evoking the in vivo imaging and synergistic dynamic therapy in tumor tissue. Mechanistically, the excess reactive oxygen species in TME can trigger the chemically initiated singlet/triplet electron exchange between the hydrophobic CDs‐Ce6 and peroxalate‐derived 1,2‐dioxetanes and thus the excess excited singlet/triplet electron of the CDs‐Ce6 can ensure the long‐persistent near‐infrared CL, type I/II photochemical production of hydroxyl radicals, superoxide radical and singlet oxygen, and type III photochemical damage of maladjusted biomacromolecules, enabling the long‐persistent near‐infrared biological imaging and enhanced cancer therapy. These results shed a new sight into the energy transfer mechanism in chemiluminescence and pave a new sight into the architecture of multifunctional theragnostic nanoplatforms.https://doi.org/10.1002/advs.202411898biological imagingcarbon nanodotschemiluminescencephotodynamic therapytriplet electron exchange
spellingShingle Run‐Wei Song
Tian‐Ci Jiang
Xue‐Yang Zhang
Cheng‐Long Shen
Qing Lou
Chong‐Xin Shan
Triplet Electron Exchange in Carbon Nanodots‐assisted Long‐persistent near‐infrared Chemiluminescence for Oncology Synergistic Imaging and Therapy
Advanced Science
biological imaging
carbon nanodots
chemiluminescence
photodynamic therapy
triplet electron exchange
title Triplet Electron Exchange in Carbon Nanodots‐assisted Long‐persistent near‐infrared Chemiluminescence for Oncology Synergistic Imaging and Therapy
title_full Triplet Electron Exchange in Carbon Nanodots‐assisted Long‐persistent near‐infrared Chemiluminescence for Oncology Synergistic Imaging and Therapy
title_fullStr Triplet Electron Exchange in Carbon Nanodots‐assisted Long‐persistent near‐infrared Chemiluminescence for Oncology Synergistic Imaging and Therapy
title_full_unstemmed Triplet Electron Exchange in Carbon Nanodots‐assisted Long‐persistent near‐infrared Chemiluminescence for Oncology Synergistic Imaging and Therapy
title_short Triplet Electron Exchange in Carbon Nanodots‐assisted Long‐persistent near‐infrared Chemiluminescence for Oncology Synergistic Imaging and Therapy
title_sort triplet electron exchange in carbon nanodots assisted long persistent near infrared chemiluminescence for oncology synergistic imaging and therapy
topic biological imaging
carbon nanodots
chemiluminescence
photodynamic therapy
triplet electron exchange
url https://doi.org/10.1002/advs.202411898
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