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Classical/Non-classical Polyoxometalate Hybrids.

ABSTRACT: Two polyanions [Se^I?V₂ Pd^II₄ W^VI₁₄ O₅₆ H]^11- and [Se^I?V₄ Pd^II₄ W^VI₂₈ O₁₀₈ H₁₂ ]^12- are the first hybrid polyoxometalates in which classical (Group?5/6 metal based) and non-classical (late transition-metal based) polyoxometalate units are joined. Requiring no supporting groups, this co-condensation of polyoxotungstate and isopolyoxopalladate constituents also provides a logical link between POM-Pd^II coordination complexes and the young subclass of polyoxopalladates. Solid-state, solution, and gas-phase studies suggest interesting specific reactivities for these hybrids and point to several potential derivatives and functionalization strategies.

SUBMITTER: Izarova NV

PROVIDER: S-EPMC5095796 | biostudies-literature | 2016 Nov

REPOSITORIES: biostudies-literature

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Classical/Non-classical Polyoxometalate Hybrids.

Izarova Natalya V NV Santiago-Schübel Beatrix B Willbold Sabine S Heß Volkmar V Kögerler Paul P

Chemistry (Weinheim an der Bergstrasse, Germany) 20161005 45

Two polyanions [SeI V2 PdII4 WVI14 O56 H]11- and [SeI V4 PdII4 WVI28 O108 H12 ]12- are the first hybrid polyoxometalates in which classical (Group 5/6 metal based) and non-classical (late transition-metal based) polyoxometalate units are joined. Requiring no supporting groups, this co-condensation of polyoxotung ...[more]

PMID: 27617918

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Project description:BACKGROUND:SOX transcription factors constitute an attractive target class for intervention with small molecules as they play a prominent role in the field of regenerative biomedicine and cancer biology. However, rationally engineering specific inhibitors that interfere with transcription factor DNA interfaces continues to be a monumental challenge in the field of transcription factor chemical biology. Polyoxometalates (POMs) are inorganic compounds that were previously shown to target the high-mobility group (HMG) of SOX proteins at nanomolar concentrations. In continuation of this work, we carried out an assessment of the selectivity of a panel of newly synthesized organo-polyoxometalate hybrids in targeting different transcription factor families to enable the usage of polyoxometalates as specific SOX transcription factor drugs. RESULTS:The residual DNA-binding activities of 15 different transcription factors were measured after treatment with a panel of diverse polyoxometalates. Polyoxometalates belonging to the Dawson structural class were found to be more potent inhibitors than the Keggin class. Further, organically modified Dawson polyoxometalates were found to be the most potent in inhibiting transcription factor DNA binding activity. The size of the polyoxometalates and its derivitization were found to be the key determinants of their potency. CONCLUSION:Polyoxometalates are highly potent, nanomolar range inhibitors of the DNA binding activity of the Sox-HMG family. However, binding assays involving a limited subset of structurally diverse polyoxometalates revealed a low selectivity profile against different transcription factor families. Further progress in achieving selectivity and deciphering structure-activity relationship of POMs require the identification of POM binding sites on transcription factors using elaborate approaches like X-ray crystallography and multidimensional NMR. In summary, our report reaffirms that transcription factors are challenging molecular architectures and that future polyoxometalate chemistry must consider further modification strategies, to address the substantial challenges involved in achieving target selectivity.

Dataset Information

Classical/Non-classical Polyoxometalate Hybrids.

Publications

Classical/Non-classical Polyoxometalate Hybrids.

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