Supramolecular Photosensitizer Enables Oxygen-Independent Generation of Hydroxyl Radicals for Photodynamic Therapy

Journal of the American Chemical Society, Journal Year: 2023, Volume and Issue: 145(7), P. 4081 - 4087

Published: Feb. 13, 2023

The highly oxygen-dependent nature of photodynamic therapy (PDT) limits its therapeutic efficacy against hypoxic solid tumors in clinics, which is an urgent problem to be solved. Herein, we develop oxygen-independent supramolecular agent that produces hydroxyl radical (•OH) by oxidizing water the presence intracellularly abundant pyruvic acid under oxygen-free conditions. A fluorene-substituted BODIPY was designed as electron donor and coassembled with perylene diimide acceptor form quadruple hydrogen-bonded agent. Detailed mechanism studies reveal intermolecular transfer charge separation upon light irradiation result efficient generation ion pairs. Under conditions, cationic radicals directly oxidize generate cytotoxic •OH, anionic electrons acid, realizing catalytic cycle. Thus, this exhibited superb photocytotoxicity even severe environments excellent vivo antitumor on HeLa-bearing mouse models. This work provides a strategy for constructing agents, opens up avenue effective PDT tumors.

Language: Английский

---

A dynamic assembly-induced emissive system for advanced information encryption with time-dependent security

Nature Communications, Journal Year: 2022, Volume and Issue: 13(1)

Published: July 20, 2022

Abstract The development of advanced materials for information encryption with time-dependent features is essential to meet the increasing demand on security. Herein, smart orthogonal and temporal properties are successfully developed based a dynamic assembly-induced multicolour supramolecular system. Multicolour fluorescence, including blue, orange even white light emissions, achieved by controlling assembly pyrene derivatives tailoring solvent composition. By taking advantage tuneable dynamically controlled functions, e.g., 3D codes, developed. Moreover, materials, such as multi-information displays 4D also enabling fluorescence-controllable system in solid phase, showing multiple pieces time scale, correct can be identified only at specified time. This work provides an inspiring point design higher security requirements.

Language: Английский

---

BODIPY as a Multifunctional Theranostic Reagent in Biomedicine: Self‐Assembly, Properties, and Applications

Advanced Materials, Journal Year: 2022, Volume and Issue: 35(18)

Published: Nov. 18, 2022

Abstract The use of boron dipyrromethene (BODIPY) in biomedicine is reviewed. To open, its synthesis and regulatory strategies are summarized, inspiring cutting‐edge work post‐functionalization highlighted. A brief overview assembly model BODIPY then provided: introduced as a promising building block for the formation single‐ multicomponent self‐assembled systems, including nanostructures suitable aqueous environments, thereby showing great development potential supramolecular applications. frontier progress biomedical application thereafter described, supported by examples frontiers applications BODIPY‐containing smart materials: it mainly involves materials based on blocks their assemblies fluorescence bioimaging, photoacoustic imaging, disease treatment photodynamic therapy, photothermal immunotherapy. Lastly, not only current status family field but also challenges worth considering summarized. At same time, insights into future prospects biomedically applicable provided.

Language: Английский

---

Integration of TADF Photosensitizer as “Electron Pump” and BSA as “Electron Reservoir” for Boosting Type I Photodynamic Therapy

Journal of the American Chemical Society, Journal Year: 2023, Volume and Issue: 145(14), P. 8130 - 8140

Published: March 31, 2023

Type I photosensitization provides an effective solution to the problem of unsatisfactory photodynamic therapeutic (PDT) effects caused by tumor hypoxia. The challenge in development mode is boost photosensitizer's own electron transfer capacity. Herein, we found that use bovine serum albumin (BSA) encapsulate a thermally activated delayed fluorescence (TADF) photosensitizer PS can significantly promote PDT process generate mass superoxide anions (O2•–). This opened new strategy employing BSA as "electron reservoir" and TADF pump". We integrated these roles one system preparing nanophotosensitizer PS@BSA. performance was demonstrated with cells under hypoxic conditions. Furthermore, PS@BSA took full advantage tumor-targeting role achieved efficient for tumor-bearing mice vivo experiments. work route improve efficiency tumors.

Language: Английский

---

Supramolecular photodynamic agents for simultaneous oxidation of NADH and generation of superoxide radical

Nature Communications, Journal Year: 2022, Volume and Issue: 13(1)

Published: Oct. 19, 2022

Abstract Given that Type-I photosensitizers (PSs) have hypoxia tolerance, developing general approaches to prepare PSs is of great importance, but remains a challenge. Here, we report supramolecular strategy for the preparation photodynamic agents, which simultaneously generate strong oxidizing cationic radicals and superoxide radicals, by introducing electron acceptors existing Type-II PSs. As proof-of-concept, three were designed co-assembled with classical PS produce quadruple hydrogen-bonded agents. The photo-induced transfer from adjacent acceptor occurs efficiently, leading generation +• an anionic radical acceptor, further transfers oxygen form O 2 −• . In addition, these agents induce direct photocatalytic oxidation NADH turnover frequency as high 53.7 min −1 , offers oxygen-independent mechanism damage tumors.

Language: Английский

---

Ruthenium-Based Photoactivated Chemotherapy

Journal of the American Chemical Society, Journal Year: 2023, Volume and Issue: 145(43), P. 23397 - 23415

Published: Oct. 17, 2023

Ruthenium(II) polypyridyl complexes form a vast family of molecules characterized by their finely tuned photochemical and photophysical properties. Their ability to undergo excited-state deactivation via photosubstitution reactions makes them quite unique in inorganic photochemistry. As consequence, they have been used, general, for building dynamic molecular systems responsive light but, more particularly, the field oncology, as prodrugs new cancer treatment modality called photoactivated chemotherapy (PACT). Indeed, coordination bond be selectively broken under visible irradiation offers fascinating perspectives oncology: it is possible make poorly toxic agents dark that become activated toward cell killing simple compound inside tumor. In this Perspective, we review most important concepts behind PACT idea, relationship between ruthenium compounds used those related phototherapeutic approach photodynamic therapy (PDT), discuss questions about real-life applications clinic. We conclude Perspective with challenges an outlook.

Language: Английский

---

Research advances in BODIPY-assembled supramolecular photosensitizers for photodynamic therapy

Coordination Chemistry Reviews, Journal Year: 2023, Volume and Issue: 496, P. 215367 - 215367

Published: Aug. 25, 2023

Language: Английский

---

Aging, oxidative stress and degenerative diseases: mechanisms, complications and emerging therapeutic strategies

Biogerontology, Journal Year: 2023, Volume and Issue: 24(5), P. 609 - 662

Published: July 30, 2023

Language: Английский

---

Ultra‐Small Nano‐Assemblies as Tumor‐Targeted and Renal Clearable Theranostic Agent for Photodynamic Therapy

Advanced Materials, Journal Year: 2023, Volume and Issue: 35(19)

Published: March 2, 2023

It is a challenge to design photosensitizers balance between the tumor-targeting enrichment for precise treatment and efficient clearance within reasonable timescale reducing side effects. Herein, an ultra-small nano-photosensitizer 1a with excellent tumor-specific accumulation renal reported. formed from self-assembly of compound 1 bearing three triethylene glycol (TEG) arms two pyridinium groups in water. The positively charged surface neutral TEG coating enables efficiently target tumor, signal-to-background ratio reaching as high 11.5 after tail intravenous injection. size average diameter 5.6 nm allows its fast through kidney. Self-assembly also endows 18.2-fold enhancement reactive oxygygen species generation rate compared organic solution. Nano-PS manifests photodynamic therapy efficacy on tumor-bearing mouse models. This work provides promising strategy clearable ability.

Language: Английский

---

Supramolecular polymers: Recent advances based on the types of underlying interactions

Progress in Polymer Science, Journal Year: 2022, Volume and Issue: 137, P. 101635 - 101635

Published: Dec. 14, 2022

Language: Английский

---