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Caging and photo-triggered uncaging of singlet oxygen by excited state engineering of electron donor-acceptor-linked molecular sensors.

ABSTRACT: Singlet oxygen (¹O₂), one of the most sought-after species in oxidative chemical reactions and photodynamic cancer therapy, is activated and neutralized in the atmosphere and living cells. It is essential to see "when" and "where" ¹O₂ is produced and delivered to understand and utilize it. There is an increasing demand for molecular sensor tools to capture, store, and supply ¹O₂, controlled by light and engineered singlet and triplet states, indicating the ¹O₂-capturing-releasing state. Here, we demonstrate the outstanding potential of an aminocoumarin-methylanthracene-based electron donor-acceptor molecule (1). Spectroscopic measurements confirm the formation of an endoperoxide (1-O₂) which is not strongly fluorescent and remarkably different from previously reported ¹O₂ sensor molecules. Moreover, the photoexcitation on the dye in 1-O₂ triggers fluorescence enhancement by the oxidative rearrangement and a competing ¹O₂ release. The unique ability of 1 will pave the way for the spatially and temporally controlled utilization of ¹O₂ in various areas such as chemical reactions and phototherapies.

SUBMITTER: Sasikumar D

PROVIDER: S-EPMC9256616 | biostudies-literature | 2022 Jul

REPOSITORIES: biostudies-literature

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Caging and photo-triggered uncaging of singlet oxygen by excited state engineering of electron donor-acceptor-linked molecular sensors.

Sasikumar Devika D Takano Yuta Y Zhao Hanjun H Kohara Reiko R Hamada Morihiko M Kobori Yasuhiro Y Biju Vasudevanpillai V

Scientific reports 20220705 1

Singlet oxygen (1O2), one of the most sought-after species in oxidative chemical reactions and photodynamic cancer therapy, is activated and neutralized in the atmosphere and living cells. It is essential to see "when" and "where" 1O2 is produced and delivered to understand and utilize it. There is an increasing demand for molecular sensor tools to capture, store, and supply 1O2, controlled by light and engineered singlet and trip ...[more]

PMID: 35790770

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Project description:Microbially-mediated uranium bioremediation has been demonstrated in uranium contaminated aquifers when acetate was artificially supplied and growth of the natural population of Geobacteraceae was stimulated. In order to mimic the environmental response to acetate, steady-state cells of G. sulfureducens were cultured in chemostats under conditions of either 1) acetate as the sole electron donor and limiting factor and fumarate as the sole electron acceptor or 2) acetate was supplied in excess with fumarate as sole electron acceptor and limiting factor. In silico fluxome modeling and transcriptome analysis were used as tools for investigating the cell response to the acetate availability. For global gene expression profiling, a DNA microarray of the complete G. sulfurreducens genome was used. Statistically significant results were obtained from two-color, dye swap hybridizations produced from a total of three biological replicates. Eight technical replicates were tested from two of the biological replicates and six technical replicates were tested from the third biological replicate. Major findings from this study are given as follows. The in silico model successfully predicted a higher TCA-cycle flux (ca. 2-fold) under acetate-excess conditions, suggesting that catabolism of acetate is favored with respect to anabolism, and thus more electrons are available for metal reduction. Transcriptome analyses offered a comprehensive picture of the regulation points subjected to the acetate availability. Under acetate-excess conditions, acetate transporters in the G. sulfurreducens genome were down-regulated. In addition the oxidation-related acetyl-CoA transferase was up-regulated approximately three-fold and the assimilatory-related acetate kinase was down-regulated approximately two-fold, respectively, indicating that the transcriptional regulation of acetate activation may be the key point for coping with the excess of acetate and increasing the TCA flux. The level of transcription for 10 c-type cytochromes was significantly increased in cells cultured with an excess of acetate. OmcS, an outer-membrane cytochrome which actively participates in electron transfer to Fe(III)-oxides and graphite electrodes from fuel cells, showed one of the highest fold increases in transcription. The integration of in silico modeling and genome-wide analysis shows for first time how G. sulffureducens adapts its metabolic flux and transcriptional network for optimizing the use of acetate as an electron donor for exocellular respiration instead of for use as a carbon source for biomass production. Keywords: Geobacter, gene expression, acetate limitation, fumarate limitation

Dataset Information

Caging and photo-triggered uncaging of singlet oxygen by excited state engineering of electron donor-acceptor-linked molecular sensors.

Publications

Caging and photo-triggered uncaging of singlet oxygen by excited state engineering of electron donor-acceptor-linked molecular sensors.

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