Photocatalytic therapy for hypoxic tumors often suffers from inefficiencies due to its dependence on oxygen and the risk of uncontrolled activation. Inspired by the oxygen-independent and precisely regulated photocatalytic functions of natural light-harvesting chlorosomes, chlorosome-mimetic nanoreactors, termed Ru-Chlos, are engineered by confining the aggregation of photosensitive ruthenium-polypyridyl-silane monomers. These Ru-Chlos exhibit markedly enhanced photocatalytic performance compared to their monomeric counterparts under acidic conditions, while notably bypassing the consumption of oxygen or hydrogen peroxide. The photocatalytic activity of Ru-Chlos is finely tunable through light-responsive disassembly of the Ru-bridged matrix, with tunability governed by pre-irradiation duration. Utilization of Ru-Chlos loading prodrug [2,2'-azino-bis(3-ethylbenzothiazoline-6-sulfonic acid)] (ABTS) for phototherapy facilitates the generation of toxic radicals (oxABTS) and the photocatalytic conversion of endogenous NADH to NAD, inducing oxidative stress in hypoxic cancer cells. Simultaneously, the light-responsive degradation of Ru-Chlos produces Ru-based toxins that further contribute to the therapeutic effect. This dual-action mechanism elicits potent immunogenic cell death effects and significantly enhances antitumor efficacy with the aid of a PD-l blockade. These biomimetic chlorosomes highlight their potential to advance oxygen-independent photocatalytic nanoreactors with controlled activity for novel cancer photoimmunotherapy strategies.
Download full-text PDF |
Source |
|---|---|
| http://dx.doi.org/10.1002/adma.202413385 | DOI Listing |
Publication Analysis
Top Keywords
Similar Publications
Biomimetic Chlorosomes: Oxygen-Independent Photocatalytic Nanoreactors for Efficient Combination Photoimmunotherapy.
Adv Mater
November 2024
State Key Laboratory of Fine Chemicals, School of Chemical Engineering, Dalian University of Technology, Dalian, 116024, China.
Photocatalytic therapy for hypoxic tumors often suffers from inefficiencies due to its dependence on oxygen and the risk of uncontrolled activation. Inspired by the oxygen-independent and precisely regulated photocatalytic functions of natural light-harvesting chlorosomes, chlorosome-mimetic nanoreactors, termed Ru-Chlos, are engineered by confining the aggregation of photosensitive ruthenium-polypyridyl-silane monomers. These Ru-Chlos exhibit markedly enhanced photocatalytic performance compared to their monomeric counterparts under acidic conditions, while notably bypassing the consumption of oxygen or hydrogen peroxide.
View Article and Find Full Text PDFEfficient two-step excitation energy transfer in artificial light-harvesting antenna based on bacteriochlorophyll aggregates.
J Photochem Photobiol B
May 2024
Department of Chemical Physics and Optics, Faculty of Mathematics and Physics, Charles University, Prague, Czech Republic. Electronic address:
Article Synopsis
- Chlorosomes in green photosynthetic bacteria help these organisms thrive in low-light conditions by efficiently harvesting light using self-organizing bacteriochlorophylls.
- Researchers created an artificial light-harvesting antenna using bacteriochlorophyll c, β-carotene, and bacteriochlorophyll a, which effectively transfers energy among these components.
- The study found that energy transfer efficiency between these pigments varied, with β-carotene content affecting the distances involved, and also developed methods to measure energy transfer that could apply to studying natural pigment complexes.
Bioinspired supramolecular nanosheets of zinc chlorophyll assemblies.
Sci Rep
October 2019
Graduate School of Life Sciences, Ritsumeikan University, Kusatsu, Shiga, 525-8577, Japan.
Two-dimensional sheet-like supramolecules have attracted much attention from the viewpoints of their potential application as functional (nano)materials due to unique physical and chemical properties. One of the supramolecular sheet-like nanostructures in nature is visible in the self-assemblies of bacteriochlorophyll-c-f pigments inside chlorosomes, which are major components in the antenna systems of photosynthetic green bacteria. Herein, we report artificial chlorosomal supramolecular nanosheets prepared by the self-assembly of a synthetic zinc 3-methoxy-chlorophyll derivative having amide and urea groups in the substituent at the 17-position.
View Article and Find Full Text PDFHeterodimers of zinc and free-base chlorophyll derivatives co-assembled in biomimetic chlorosomal J-aggregates.
Photochem Photobiol Sci
February 2019
Graduate School of Life Sciences, Ritsumeikan University, Kusatsu, Shiga, 525-8577, Japan.
Light-harvesting antennas are one of the most important types of apparatus that use solar energy for natural and artificial photosynthesis. Bacteriochlorophyll (BChl) and chlorophyll (Chl) pigments play key roles in absorbing photons from the sun, migrating/transferring the singlet excitation energy, and transferring electrons. Chlorosomes, the main light-harvesting antennas of photosynthetic green bacteria, contain self-aggregates composed of a large number of BChl-c, d, e, and f molecules without any assistance from peptides, and such J-aggregates transfer the harvested energy to BChl-a pigments of baseplate proteins.
View Article and Find Full Text PDFPhototriggered Dynamic and Biomimetic Growth of Chlorosomal Self-Aggregates.
J Am Chem Soc
January 2019
Graduate School of Life Sciences , Ritsumeikan University, Kusatsu , Shiga 525-8577 , Japan.
Supramolecular polymerizations mimicking native systems, which are step-by-step constructions to form self-aggregates, were recently developed. However, a general system to successively and spontaneously form self-aggregates from monomeric species remains challenging. Here, we report a photoinduced supramolecular polymerization system as a biomimetic formation of chlorophyll aggregates which are the main light-harvesting antennas in photosynthetic green bacteria, called "chlorosomes".
View Article and Find Full Text PDFWant AI Summaries of new PubMed Abstracts delivered to your In-box?
Enter search terms and have AI summaries delivered each week - change queries or unsubscribe any time!