Dataset Information

New Photosensitizers Based on Heteroleptic CuI Complexes and CO2 Photocatalytic Reduction with [NiII (cyclam)]Cl2.

ABSTRACT: Earth-abundant metal complexes have been attracting increasing attention in the field of photo(redox)catalysis. In this work, the synthesis and full characterisation of four new heteroleptic CuI complexes are reported, which can work as photosensitizers. The complexes bear a bulky diphosphine (DPEPhos=bis[(2-diphenylphosphino)phenyl] ether) and a diimine chelating ligand based on 1-benzyl-4-(quinol-2'yl)-1,2,3-triazole. Their absorption has a relative maximum in the visible-light region, up to 450?nm. Thus, their use in photocatalytic systems for the reduction of CO2 with blue light in combination with the known catalyst [NiII (cyclam)]Cl2 was tested. This system produced CO as the main product through visible light (?=420?nm) with a TON up to 8 after 4?hours. This value is in line with other photocatalytic systems using the same catalyst. Nevertheless, this system is entirely noble-metal free.

SUBMITTER: Gracia LL

PROVIDER: S-EPMC7497214 | biostudies-literature | 2020 Jul

REPOSITORIES: biostudies-literature

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New Photosensitizers Based on Heteroleptic CuI Complexes and CO2 Photocatalytic Reduction with [NiII (cyclam)]Cl2.

Gracia Lisa-Lou LL Luci Luisa L Bruschi Cecilia C Sambri Letizia L Weis Patrick P Fuhr Olaf O Bizzarri Claudia C

Chemistry (Weinheim an der Bergstrasse, Germany) 20200716 44

Earth-abundant metal complexes have been attracting increasing attention in the field of photo(redox)catalysis. In this work, the synthesis and full characterisation of four new heteroleptic CuI complexes are reported, which can work as photosensitizers. The complexes bear a bulky diphosphine (DPEPhos=bis[(2-diphenylphosphino)phenyl] ether) and a diimine chelating ligand based on 1-benzyl-4-(quinol-2'yl)-1,2,3-triazole. Their absorption has a relative maximum in the visible-light regi ...[more]

PMID: 32672408

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Project description:BackgroundDiacetyl-bis(N4-methylthiosemicarbazone), labeled with 64Cu (64Cu-ATSM) has been suggested as a promising tracer for imaging hypoxia. However, various controversial studies highlighted potential pitfalls that may disable its use as a selective hypoxic marker. They also highlighted that the results may be tumor location dependent. Here, we first analyzed uptake of Cu-ATSM and its less lipophilic counterpart Cu-Cl2 in the tumor over time in an orthotopic glioblastoma model. An in vitro study was also conducted to investigate the hypoxia-dependent copper uptake in tumor cells. We then further performed a comprehensive ex vivo study to compare 64Cu uptake to hypoxic markers, specific cellular reactions, and also transporter expression.MethodsμPET was performed 14 days (18F-FMISO), 15 days (64Cu-ATSM and 64Cu-Cl2), and 16 days (64Cu-ATSM and 64Cu-Cl2) after C6 cell inoculation. Thereafter, the brains were withdrawn for further autoradiography and immunohistochemistry. C6 cells were also grown in hypoxic workstation to analyze cellular uptake of Cu complexes in different oxygen levels.ResultsIn vivo results showed that Cu-ASTM and Cu-Cl2 accumulated in hypoxic areas of the tumors. Cu-ATSM also stained, to a lesser extent, non-hypoxic regions, such as regions of astrogliosis, with high expression of copper transporters and in particular DMT-1 and CTR1, and also characterized by the expression of elevated astrogliosis. In vitro results show that 64Cu-ATSM showed an increase in the uptake only in severe hypoxia at 0.5 and 0.2% of oxygen while for 64Cu-Cl2, the cell retention was significantly increased at 5% and 1% of oxygen with no significant rise at lower oxygen percentages.ConclusionIn the present study, we show that Cu-complexes undoubtedly accumulate in hypoxic areas of the tumors. This uptake may be the reflection of a direct dependency to a redox metabolism and also a reflection of hypoxic-induced overexpression of transporters. We also show that Cu-ATSM also stained non-hypoxic regions such as astrogliosis.

Dataset Information

New Photosensitizers Based on Heteroleptic CuI Complexes and CO2 Photocatalytic Reduction with [NiII (cyclam)]Cl2.

Publications

New Photosensitizers Based on Heteroleptic Cu<sup>I</sup> Complexes and CO<sub>2</sub> Photocatalytic Reduction with [Ni<sup>II</sup> (cyclam)]Cl<sub>2</sub>.

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