ACS Materials Letters, Journal Year: 2025, Volume and Issue: unknown, P. 1887 - 1895
Published: April 16, 2025
Language: Английский
Advanced Materials, Journal Year: 2025, Volume and Issue: unknown
Published: Jan. 26, 2025
Abstract Photodynamic therapy (PDT) using traditional type II photosensitizers (PSs) has been limited in hypoxic tumors due to excessive oxygen consumption. The conversion from into a less oxygen‐dependent I PDT pathway shown the potential combat tumors. Herein, design of heterodimeric PS, NBSSe , by conjugating widely used PS NBS and NBSe via molecular dimerization, achieving aggregation‐regulated efficient photodynamic for first time is reported. Electrochemistry characterizations theoretical calculations elucidate that tends form S +· /Se −· radical pair intramolecular electron transfer co‐excited * aggregate, realizing 7.25‐fold O 2 generation compared 80% suppression 1 . enhanced enables excellent anti‐hypoxia efficiency inhibition pulmonary metastasis. Additionally, incorporation electron‐rich bovine serum albumin accelerates recycling cationic further boosting photostability generation. resultant BSA@NBSSe nanoparticles demonstrate successful tumor‐targeting capability. This work provides an appealing avenue convert ROS cancer phototherapy hypoxia.
Language: Английский
Citations
3
Advanced Materials, Journal Year: 2024, Volume and Issue: unknown
Published: Aug. 3, 2024
Compared with conventional therapies, photoimmunotherapy offers precise targeted cancer treatment minimal damage to healthy tissues and reduced side effects, but its efficacy may be limited by shallow light penetration the potential for tumor resistance. Here, an acceptor-donor-acceptor (A-D-A)-structured nanoaggregate is developed dual phototherapy, including photodynamic therapy (PDT) photothermal (PTT), triggered single near-infrared (NIR) light. Benefiting from strong intramolecular charge transfer (ICT), A-D-A-structured nanoaggregates exhibit broad absorption extending NIR region effectively suppressed fluorescence, which enables deep efficient conversion (η = 67.94%). A suitable HOMO-LUMO distribution facilitates sufficient intersystem crossing (ISC) convert ground-state oxygen (
Language: Английский
Citations
16
Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(47)
Published: July 31, 2024
Abstract Near‐infrared photosensitizers are valuable tools to improve treatment depth in photodynamic therapy (PDT). However, their low singlet oxygen ( 1 O 2 ) generation ability, indicated by quantum yield, presents a formidable challenge for PDT. To overcome this challenge, the heptamethine cyanine was decorated with biocompatible S Scy7 and Se Secy7 atom. We observe that exhibits redshift main absorption ~840 nm an ultra‐efficient capacity. The emergence of strong intramolecular charge transfer effect between atom polymethine chain considerably narrows energy gap (0.51 eV), heavy strengthens spin–orbit coupling (1.44 cm −1 ), both which greatly improved high triplet state yield (61 %), determines . Therefore, demonstrated excellent capacity, is ~24.5‐fold indocyanine green, ~8.2‐fold IR780, ~1.3‐fold methylene blue under low‐power‐density 850 irradiation (5 mW −2 ). considerable phototoxicity toward cancer cells buried 12 mm tissue. Nanoparticles formed encapsulating within amphiphilic polymers lecithin, promising antitumor anti‐pulmonary metastatic effects, exhibiting remarkable potential advancing PDT deep tissues.
Language: Английский
Citations
14
Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 64(1)
Published: Oct. 25, 2024
Although Type-I photodynamic therapy has attracted increasingly growing interest due to its reduced dependence on oxygen, the design of effective photosensitizers remains a challenge. In this work, we report strategy for by involvement hydrogen atom transfer (HAT). As proof concept, HAT-involved PS, which simultaneously generates superoxide and carbon-centered radicals under light-irradiation, was synthesized. This photosensitizer is comprised fluorene-substituted BODIPY unit as an electron acceptor covalently linked with triphenylamine moiety donor. Under photo-induced intramolecular occurs generate anion radical cation radical. The former transfers electrons oxygen O
Language: Английский
Citations
11
Journal of Medicinal Chemistry, Journal Year: 2025, Volume and Issue: unknown
Published: Jan. 24, 2025
The hypoxic environment of solid tumors significantly diminishes the therapeutic efficacy oxygen-dependent photodynamic therapy. Developing efficient photosensitizers that operate via photoredox catalysis presents a promising strategy to overcome this challenge. Herein, we report rational design two rhenium(I) tricarbonyl complexes (Re-TPO and Re-TP) with electron donor–acceptor–donor configuration. Notably, Re-TP exhibits aggregation-induced emission properties enhanced spin–orbit coupling compared Re-TPO, thus exhibiting promoted photosensitizing capability. In addition generating type I II reactive oxygen species, excited facilitates photocatalytic oxidation NADH NAD+ photoreduction pyruvic acid lactic acid. This metabolic intervention triggers PD-L1-linked immune responses disrupts tumor redox balance, leading ferroptosis immunogenic cell death. combined immunotherapy effects suppress both primary distant B16 tumors. investigation provides compelling model for designing metal-based PSs photoredox-mediated photoimmunotherapy against
Language: Английский
Citations
2
Advanced Materials, Journal Year: 2025, Volume and Issue: unknown
Published: Feb. 9, 2025
Abstract Photodynamic therapy (PDT) holds significant promise for antibacterial treatment, with its potential markedly amplified when using Type I photosensitizers (PSs). However, developing PSs remains a challenge due to lack of reliable design strategy. Herein, PS nanocluster is developed via self‐assembly zwitterionic small molecule (C3TH) superior PDT in vivo. Mechanism studies demonstrate that unique cross‐arranged C3TH within not only shortens intermolecular distance but also inhibits electronic‐vibrational coupling, thus facilitating photoinduced electron transfer form radical cation and anion autoionization reaction. Subsequently, these highly oxidizing or reducing radicals engage cascade photoredox generate efficient ·OH O 2 ‾·. As result, nanoclusters achieve 97.6% efficacy against MRSA at an ultralow dose, surpassing the commercial antibiotic Vancomycin by more than 8.8‐fold. These findings deepen understanding PDT, providing novel strategy PSs.
Language: Английский
Citations
2
Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 64(1)
Published: Aug. 23, 2024
Chalcogens are used as sensitive redox-responsive reagents in tumor therapy. However, chalcogen bonds triggered by external ionizing radiation, rather than internal environmental stimuli, enable site-directed and real-time drug degradation target lesions. This approach helps to bypass chemoresistance global systemic toxicity, presenting a significant advancement over traditional chemoradiotherapy. In this study, we fabricated hybrid monodisperse organosilica nanoprodrug based on homonuclear single (disulfide (S-S, approximately 240 kJ/mol), diselenium (Se-Se, 172 tellurium (Te-Te, 126 kJ/mol)), including ditelluride-bond-bridged MONs (DTeMSNs), diselenide-bond-bridged (DSeMSNs) disulfide-bond-bridged (DSMSNs). The results demonstrated that differences electronegativities atomic radii influenced their oxidation sensitivities reactivities. Tellurium, with the lowest electronegativity, showed highest sensitivity, followed selenium sulfur. DTeMSNs exhibited highly responsive cleavage upon exposure X-rays, resulting TeO
Language: Английский
Citations
9
Advanced Functional Materials, Journal Year: 2024, Volume and Issue: unknown
Published: June 16, 2024
Abstract Photodynamic therapy (PDT) presents a promising approach for combating periodontitis, an infectious disease triggered by bacteria. However, the hypoxic environment within periodontal pockets poses challenges PDT efficacy. In this study, novel purine‐based C^N ligands are utilized to develop Ir(III) complexes with enhanced reactive oxygen species (ROS) generation capacity periodontitis treatment. The type I/II performance of is greatly purine ligands, which leads potent bactericidal and biofilm elimination rat model local application these effectively achieves antibacterial anti‐inflammatory effects while promoting tissue repair under clinical luminaire exposure. This strategy utilizing circumvents need antibiotics surgical intervention, emerging as promising, non‐invasive managing periodontitis.
Language: Английский
Citations
6
Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(49)
Published: Aug. 22, 2024
Abstract Carbon dots (CDs) have gained significant interest because of their potential in biomedical applications. Nevertheless, developing CDs with efficient photoinduced charge separation for tumor photodynamic therapy (PDT) remains a challenge. This study presents novel class supra‐carbon‐dots (supra‐CDs) developed by fusing red emissive 2,3‐dicyanohydroquinone (DCHQ) via post‐solvothermal treatment. In supra‐CDs, the core, acting as electron donors, is formed assembled substantial sp 2 domains, fused interface originating from DCHQ electron‐withdrawing groups functions acceptor. configuration creates unique donor‐acceptor nanostructure. Upon white light irradiation, excited electrons were transferred to interface, whereas photogenerated holes retained within radicals, leading effective separation. The separated then react oxygen generate superoxide radicals. Simultaneously, undergo oxidation crucial cellular substrates. dual action underscores exceptional cell‐killing efficacy supra‐CDs. Moreover, increased particle sizes (~20 nm) ensure supra‐CDs exhibit notable capacity accumulation improved permeability and retention effect, thereby achieving satisfactory anti‐tumor PDT mouse subcutaneous model.
Language: Английский
Citations
5
ACS Applied Materials & Interfaces, Journal Year: 2024, Volume and Issue: 16(31), P. 40428 - 40443
Published: July 23, 2024
The spin-orbit charge transfer intersystem crossing (SOCT-ISC) photophysical process has shown great potential for constructing heavy-atom-free photosensitizers (PSs) photodynamic therapy (PDT) of tumors. However, almost all such PSs reported to date, the SOCT-ISC is driven by acceptor-excited photoinduced electron (a-PeT). In this work, first time donor-excited (d-PeT)-driven mechanism utilized construct PDT tumors directly installing electron-deficient N-alkylquinolinium unit (as an acceptor) into meso-position near-infrared (NIR) distyryl Bodipy chromophore donor). less polar environment, exist as monomer and promote production singlet oxygen (1O2) (Type-II) relying on d-PeT-driven population triplet excited state via SOCT-ISC, whereas in aqueous they nanoaggregates induce generation superoxides (O2-•) hydroxyl radicals (HO•) (Type-I) formation delocalized charge-separated state. could rapidly be internalized cancer cells simultaneous intracellular 1O2, O2-•, HO• upon NIR light irradiation, endowing with superb photocytotoxicity IC50 values up submicromolar levels whether under normoxia or hypoxia. Based platform, a tumor-targetable PS developed, its abilities killing ablating without damage normal cells/tissues irradiation are verified vitro vivo. study expands design scope introducing d-PeT conception, thus being highly valuable achieving novel realm tumor PDT.
Language: Английский
Citations
4