Thymoquinone as an electron transfer mediator to convert Type II photosensitizers to Type I photosensitizers DOI Creative Commons
Jiahao Zhuang, Guobin Qi,

Yecheng Feng

et al.

Nature Communications, Journal Year: 2024, Volume and Issue: 15(1)

Published: June 10, 2024

Abstract The development of Type I photosensitizers (PSs) is great importance due to the inherent hypoxic intolerance photodynamic therapy (PDT) in microenvironment. Compared II PSs, PSs are less reported absence a general molecular design strategy. Herein, we report that combination typical PS and natural substrate carvacrol (CA) can significantly facilitate pathway efficiently generate superoxide radical (O 2 –• ). Detailed mechanism study suggests CA activated into thymoquinone (TQ) by local singlet oxygen generated from upon light irradiation. With TQ as an efficient electron transfer mediator, it promotes conversion O via transfer-based pathway. Notably, three classical employed demonstrate universality proposed approach. PDT against S. aureus has been demonstrated under conditions vitro. Furthermore, this coupled agent exhibits significant bactericidal activity with antibacterial rate 99.6% for bacterial-infection female mice vivo experiments. Here, show simple, effective, universal method endow traditional tolerance.

Language: Английский

Recent advances in type I organic photosensitizers for efficient photodynamic therapy for overcoming tumor hypoxia DOI
Bingli Lu, Lingyun Wang, Hao Tang

et al.

Journal of Materials Chemistry B, Journal Year: 2023, Volume and Issue: 11(21), P. 4600 - 4618

Published: Jan. 1, 2023

Photodynamic therapy (PDT) with an oxygen-dependent character is a noninvasive therapeutic method for cancer treatment.

Language: Английский

Citations

59
Oxygen-independent organic photosensitizer with ultralow-power NIR photoexcitation for tumor-specific photodynamic therapy DOI Creative Commons
Yufu Tang, Yuanyuan Li, Bowen Li

et al.

Nature Communications, Journal Year: 2024, Volume and Issue: 15(1)

Published: March 21, 2024

Abstract Photodynamic therapy (PDT) is a promising cancer treatment but has limitations due to its dependence on oxygen and high-power-density photoexcitation. Here, we report polymer-based organic photosensitizers (PSs) through rational PS skeleton design precise side-chain engineering generate •O 2 − •OH under oxygen-free conditions using ultralow-power 808 nm photoexcitation for tumor-specific photodynamic ablation. The designed skeletons can electron-hole pairs sensitize H O into with photoexcitation, achieving NIR-photoexcited oxygen-independent production. Further, compared commonly used alkyl side chains, glycol oligomer as the chain mitigates recombination offers more molecules around generated from hydrophobic skeletons, which yield 4-fold stronger production, thus allowing an high PDT effect. Finally, feasibility of developing activatable PSs in female mice further demonstrated irradiation 15 mW cm −2 . study not only provides insights mechanism also general guideline develop NIR PDT.

Language: Английский

Citations

59
Near-Infrared-II-Activatable Self-Assembled Manganese Porphyrin-Gold Heterostructures for Photoacoustic Imaging-Guided Sonodynamic-Augmented Photothermal/Photodynamic Therapy DOI

Peijing Xu,

Changchun Wen, Cunji Gao

et al.

ACS Nano, Journal Year: 2023, Volume and Issue: 18(1), P. 713 - 727

Published: Dec. 20, 2023

Porphyrins and their derivatives are widely used as photosensitizers sonosensitizers in tumor treatment. Nevertheless, poor water solubility low chemical stability reduce singlet oxygen (1O2) yield and, consequently, photodynamic therapy (PDT) sonodynamic (SDT) efficiency. Although strategies for porphyrin molecule assembly have been developed to augment 1O2 generation, there is scope further improving PDT SDT efficiencies. Herein, we synthesized ordered manganese (SM) nanoparticles with well-defined self-assembled metalloporphyrin networks that enabled efficient energy transfer enhanced photocatalytic sonocatalytic activity production. Subsequently, Au were grown situ on the SM surface by anchoring terminal alkynyl of form plasmonic SMA heterostructures, which showed excellent near-infrared-II (NIR-II) region absorption photothermal properties, facilitated electron–hole pair separation transfer. With modification hyaluronic acid (HA), SMAH heterostructure nanocomposites exhibited good actively targeted cancer cells. Under NIR-II light ultrasound (US) irradiation, generates hyperthermia, a large amount 1O2, inducing cell damage. Both vitro vivo studies confirmed effectively suppressed growth decreasing GSH levels SDT-augmented PDT/PTT. Moreover, utilizing strong window, can achieve photoacoustic imaging-guided combined This work provides paradigm enhancing metalloporphyrins improve synergistic therapeutic effect SDT/PDT/PTT.

Language: Английский

Citations

56
A Metal‐Free Mesoporous Carbon Dots/Silica Hybrid Type I Photosensitizer with Enzyme‐Activity for Synergistic Treatment of Hypoxic Tumor DOI
Boshi Tian, Shaohua Liu, Chenghao Yu

et al.

Advanced Functional Materials, Journal Year: 2023, Volume and Issue: 33(25)

Published: March 10, 2023

Abstract As a less O 2 ‐dependent photodynamic therapy (PDT), type I PDT is an effective approach to overcome the hypoxia‐induced low efficiency against solid tumors. However, commonly used metal‐involved agents suffer from long‐term biosafety concern. Herein, metal‐free photosensitizer, N ‐doped carbon dots/mesoporous silica nanoparticles (NCDs/MSN, ≈40 nm) nanohybrid with peroxidase (POD)‐like activity for synergistic and enzyme‐activity treatment, developed on gram scale via facile one‐pot strategy through mixing source precursor assistance of template. Benefiting narrow bandgap (1.92 eV) good charge separation capacity NCDs/MSN, upon 640 nm light irradiation, excited electrons in conduction band can effectively generate •− by reduction dissolved one‐electron transfer process even under hypoxic conditions, inducing apoptosis tumor cells. Moreover, photoinduced partially transform into more toxic • OH two‐electron reduction. POD‐like NCDs/MSN catalyze endogenous H microenvironment, further synergistically ablating 4T1 Therefore, mass production way synthesize novel photosensitizer enzyme‐mimic treatment tumors provided, which exhibits promising clinical translation prospects.

Language: Английский

Citations

55
Photo‐Induced Disproportionation‐Mediated Photodynamic Therapy: Simultaneous Oxidation of Tetrahydrobiopterin and Generation of Superoxide Radicals DOI
Kun‐Xu Teng, Dongsheng Zhang,

Bin‐Kai Liu

et al.

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(12)

Published: Jan. 23, 2024

We herein present an approach of photo-induced disproportionation for preparation Type-I photodynamic agents. As a proof concept, BODIPY-based photosensitizers were rationally designed and prepared. The intermolecular electron transfer between homotypic chromophores leads to the reaction, resulting in formation charged intermediates, cationic anionic radicals. radicals efficiently oxidize cellularimportant coenzyme, tetrahydrobiopterin (BH

Language: Английский

Citations

43
Selenium‐Containing Type‐I Organic Photosensitizers with Dual Reactive Oxygen Species of Superoxide and Hydroxyl Radicals as Switch‐Hitter for Photodynamic Therapy DOI Creative Commons
Haiyang Wang, Tian Qin, Wen Wang

et al.

Advanced Science, Journal Year: 2023, Volume and Issue: 10(24)

Published: June 25, 2023

Abstract Organic type‐I photosensitizers (PSs) which produce aggressive reactive oxygen species (ROS) with less oxygen‐dependent exhibit attractive curative effect for photodynamic therapy (PDT), as they adapt better to hypoxia microenvironment in tumors. However, the reported PSs are limited and its exacted mechanism of dependence is still unclear. Herein, new selenium‐containing Se6 Se5 benzoselenadiazole acceptor has been designed possessed aggregation‐induced emission characteristic. Benefited from double heavy‐atom‐effect selenium bromine, shows a smaller energy gap (Δ E ST ) 0.03 eV improves ROS efficiency. Interestingly, radicals both long‐lived superoxide anion (O 2 •‾ short‐lived hydroxyl ( • OH) generated them upon irradiation. This may provide switch‐hitter dual‐radical complementary lifetimes PDT. More importantly, simultaneous processes OH revealed, including disproportionation O reaction between excited PS water. Actually, displays superior in–vitro PDT performance commercial chlorin e6 (Ce6), under normoxia or hypoxia. After intravenous injection, significantly in–vivo demonstrated on Se6, where tumor growth inhibition rates 99% higher than Ce6. These findings offer insights about molecular design study PSs.

Language: Английский

Citations

42
Nanocatalysts for modulating antitumor immunity: fabrication, mechanisms and applications DOI
Xianbo Wu, Yuqing Li, Mei Wen

et al.

Chemical Society Reviews, Journal Year: 2024, Volume and Issue: 53(5), P. 2643 - 2692

Published: Jan. 1, 2024

This review discusses the structures and engineering strategies of nanocatalysts, highlighting their underlying mechanisms applications in cancer immunotherapy.

Language: Английский

Citations

40
Expanded ROS Generation and Hypoxia Reversal: Excipient‐free Self‐assembled Nanotheranostics for Enhanced Cancer Photodynamic Immunotherapy DOI

Jing Yang,

Bibo Ren,

Xuntao Yin

et al.

Advanced Materials, Journal Year: 2024, Volume and Issue: 36(30)

Published: May 12, 2024

The efficacy of photodynamic therapy (PDT)-related cancer therapies is significantly restricted by two irreconcilable obstacles, i.e., low reactive oxygen species (ROS) generation capability and hypoxia which constrains the immune response. Herein, this work develops a self-assembled clinical photosensitizer indocyanine green (ICG) HSP90 inhibitor 17-dimethylaminoethylamino-17-demethoxygeldanamycin (17-DMAG) nanoparticles (ISDN) without any excipient. This discovers that hydrophobic interaction forces between ICG 17-DMAG promote photostability its intersystem crossing (ISC) process, thereby improving ROS quantum yield from 0.112 to 0.46. Augmented enhances PDT further immunogenic cell death (ICD) effects. inhibits HSP90/hypoxia-inducible factor 1α (HIF-1α) axis dramatically reverse immunosuppressive tumor microenvironment caused PDT-aggravated hypoxia. In mouse model pancreatic cancer, ISDN markedly improve cytotoxic T lymphocyte infiltration MHC I II activation, demonstrating superior ICD effects in situ powerful systematic antitumor immunity generation, eventually achieving vigorous recurrence resistance. study proposes an unsophisticated versatile strategy for enhancing systemic potentially extending it multiple cancers.

Language: Английский

Citations

34
Crucial Breakthrough of BODIPY‐Based NIR‐II Fluorescent Emitters for Advanced Biomedical Theranostics DOI
Xiaoming Hu, Zhu-ting Fang,

Caijun Zhu

et al.

Advanced Functional Materials, Journal Year: 2024, Volume and Issue: 34(36)

Published: March 29, 2024

Abstract Fluorescence imaging in the second near‐infrared window (NIR‐II, 1000–1700 nm) has aroused immense attention for biomedical applications, offering exceptional advantages such as ultra‐low photon scattering and increased tissue penetration. Among NIR‐II‐emitted organic dyes, Boron dipyrromethene (BODIPY), emerged a noteworthy candidate. BODIPY, distinguished by its controllable molecular structure optical properties, outstanding fluorescence quantum yields, high molar absorption coefficients, remarkable chemical stability, undergone comprehensive investigation extensive exploration within realm of biological theranostics. This work aims to provide summary advancements development design strategies NIR‐II BODIPY fluorophores tailored advanced phototheranostics. Initially, elucidates several representative strategies, concluding electron‐programming strategy, extension conjugated backbone, J‐aggregation strategic establishment activatable fluorophores, which enhance skeletons. Subsequently, developments fluorescent BODIPY‐based nanoplatforms applications are intricately elaborated. In conclusion, this outlines future efforts directions refining meet evolving clinical demands. It is anticipated that contribution may feasible reference thereby advancing their potential practices.

Language: Английский

Citations

25
Metallopolymer strategy to explore hypoxic active narrow-bandgap photosensitizers for effective cancer photodynamic therapy DOI Creative Commons
Zhao Zhang, Zixiang Wei,

Jintong Guo

et al.

Nature Communications, Journal Year: 2024, Volume and Issue: 15(1)

Published: Jan. 2, 2024

Abstract Practical photodynamic therapy calls for high-performance, less O 2 -dependent, long-wavelength-light-activated photosensitizers to suit the hypoxic tumor microenvironment. Iridium-based exhibit excellent photocatalytic performance, but in vivo applications are hindered by conventional -dependent Type-II photochemistry and poor absorption. Here we show a general metallopolymerization strategy engineering iridium complexes exhibiting Type-I enhancing absorption intensity blue near-infrared region. Reactive oxygen species generation of metallopolymer Ir-P1 , where atom is covalently coupled polymer backbone, over 80 times higher than that its mother without under 680 nm irradiation. This also works effectively when directly included ( Ir-P2 ) backbones, wide generality. The nanoparticles efficient •− conjugated with integrin αvβ3 binding cRGD achieve targeted therapy.

Language: Английский

Citations

24