Ca(2+)-triggered allosteric catalysts crosstalk with cellular redox systems through their foldase- and reductase-like activities

Ca(2+)触发的变构催化剂通过其折叠酶样和还原酶样活性与细胞氧化还原系统进行相互作用。

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Abstract

Effective chemical catalysts can artificially control intracellular metabolism. However, in conventional catalytic chemistry, activity and cytotoxicity have a trade-off relationship; thus, driving catalysts in living cells remains challenging. To overcome this critical issue at the interface between catalytic chemistry and biology, we developed cell-driven allosteric catalysts that exert catalytic activity at specific times. The synthesized allosteric redox catalysts up- and downregulated their foldase- and antioxidase-like activities in response to varying Ca(2+) concentrations, which is a key factor for maintenance of the redox status in cells. In the absence of Ca(2+) or at low Ca(2+) concentrations, the compounds were mostly inactive and hence did not affect cell viability. In contrast, under specific conditions with elevated cytosolic Ca(2+) concentrations, the activated compounds resisted the redox imbalance induced by the reactive oxygen species generated by Ca(2+)-stimulated mitochondria. Smart catalysts that crosstalk with biological phenomena may provide a platform for new prodrug development guidelines.

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