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Targeted photoredox catalysis in cancer cells
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Huang, Huaiyi, Banerjee, Samya, Qiu, Kangqiang, Zhang, Pingyu, Blacque, Olivier, Malcomson, Thomas, Paterson, Martin J., Clarkson, Guy J., Staniforth, Michael, Stavros, Vasilios G., Gasser, Gilles, Chao, Hui and Sadler, Peter J. (2019) Targeted photoredox catalysis in cancer cells. Nature Chemistry, 11 . pp. 1041-1048. doi:10.1038/s41557-019-0328-4 ISSN 1755-4330.
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Official URL: https://doi.org/10.1038/s41557-019-0328-4
Abstract
Hypoxic tumours are a major problem for cancer photodynamic therapy. Here, we show that photoredox catalysis can provide an oxygen-independent mechanism of action to combat this problem. We have designed a highly oxidative Ir(III) photocatalyst, [Ir(ttpy)(pq)Cl]PF ([1]PF , where 'ttpy' represents 4'-(p-tolyl)-2,2':6',2''-terpyridine and 'pq' represents 3-phenylisoquinoline), which is phototoxic towards both normoxic and hypoxic cancer cells. Complex 1 photocatalytically oxidizes 1,4-dihydronicotinamide adenine dinucleotide (NADH)-an important coenzyme in living cells-generating NAD radicals with a high turnover frequency in biological media. Moreover, complex 1 and NADH synergistically photoreduce cytochrome c under hypoxia. Density functional theory calculations reveal π stacking in adducts of complex 1 and NADH, facilitating photoinduced single-electron transfer. In cancer cells, complex 1 localizes in mitochondria and disrupts electron transport via NADH photocatalysis. On light irradiation, complex 1 induces NADH depletion, intracellular redox imbalance and immunogenic apoptotic cancer cell death. This photocatalytic redox imbalance strategy offers a new approach for efficient cancer phototherapy.
Item Type: | Journal Article | ||||||||||||||||||||||||||||||||||||||||||||||||||||||||||||
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Subjects: | R Medicine > RC Internal medicine > RC0254 Neoplasms. Tumors. Oncology (including Cancer) | ||||||||||||||||||||||||||||||||||||||||||||||||||||||||||||
Divisions: | Faculty of Science, Engineering and Medicine > Science > Chemistry | ||||||||||||||||||||||||||||||||||||||||||||||||||||||||||||
SWORD Depositor: | Library Publications Router | ||||||||||||||||||||||||||||||||||||||||||||||||||||||||||||
Library of Congress Subject Headings (LCSH): | Cancer -- Photochemotherapy, Antineoplastic agents -- Research, Catalysis, Organic compounds -- Synthesis | ||||||||||||||||||||||||||||||||||||||||||||||||||||||||||||
Journal or Publication Title: | Nature Chemistry | ||||||||||||||||||||||||||||||||||||||||||||||||||||||||||||
Publisher: | Nature Publishing Group | ||||||||||||||||||||||||||||||||||||||||||||||||||||||||||||
ISSN: | 1755-4330 | ||||||||||||||||||||||||||||||||||||||||||||||||||||||||||||
Official Date: | November 2019 | ||||||||||||||||||||||||||||||||||||||||||||||||||||||||||||
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Volume: | 11 | ||||||||||||||||||||||||||||||||||||||||||||||||||||||||||||
Page Range: | pp. 1041-1048 | ||||||||||||||||||||||||||||||||||||||||||||||||||||||||||||
DOI: | 10.1038/s41557-019-0328-4 | ||||||||||||||||||||||||||||||||||||||||||||||||||||||||||||
Status: | Peer Reviewed | ||||||||||||||||||||||||||||||||||||||||||||||||||||||||||||
Publication Status: | Published | ||||||||||||||||||||||||||||||||||||||||||||||||||||||||||||
Access rights to Published version: | Restricted or Subscription Access | ||||||||||||||||||||||||||||||||||||||||||||||||||||||||||||
Date of first compliant deposit: | 1 November 2019 | ||||||||||||||||||||||||||||||||||||||||||||||||||||||||||||
Date of first compliant Open Access: | 23 March 2020 | ||||||||||||||||||||||||||||||||||||||||||||||||||||||||||||
RIOXX Funder/Project Grant: |
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