Abstract
The discovery of inhibitors of methyl- and acetyl-binding domains has provided evidence for the 'druggability' of epigenetic effector molecules. The small-molecule probe UNC1215 prevents methyl-dependent protein-protein interactions by engaging the aromatic cage of MBT domains and, with lower affinity, Tudor domains. Using a library of tagged UNC1215 analogs, we screened a protein-domain microarray of human methyllysine effector molecules to rapidly detect compounds with new binding profiles with either increased or decreased specificity. Using this approach, we identified a compound (EML405) that acquired a novel interaction with the Tudor-domain-containing protein Spindlin1 (SPIN1). Structural studies facilitated the rational synthesis of SPIN1 inhibitors with increased selectivity (EML631-633), which engage SPIN1 in cells, block its ability to 'read' H3K4me3 marks and inhibit its transcriptional-coactivator activity. Protein microarrays can thus be used as a platform to 'target-hop' and identify small molecules that bind and compete with domain-motif interactions.
MeSH terms
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Benzamides / chemical synthesis
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Benzamides / chemistry
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Benzamides / pharmacology*
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Cell Cycle Proteins / antagonists & inhibitors*
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Cell Cycle Proteins / chemistry
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Dose-Response Relationship, Drug
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Humans
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Microtubule-Associated Proteins / antagonists & inhibitors*
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Microtubule-Associated Proteins / chemistry
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Models, Molecular
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Molecular Structure
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Phosphoproteins / antagonists & inhibitors*
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Phosphoproteins / chemistry
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Piperidines / chemical synthesis
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Piperidines / chemistry
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Piperidines / pharmacology*
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Protein Array Analysis*
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Small Molecule Libraries / chemical synthesis
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Small Molecule Libraries / chemistry
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Small Molecule Libraries / pharmacology*
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Structure-Activity Relationship
Substances
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Benzamides
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Cell Cycle Proteins
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Microtubule-Associated Proteins
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Phosphoproteins
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Piperidines
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Small Molecule Libraries
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UNC1215
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spindlin
Associated data
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PubChem-Substance/333497403
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PubChem-Substance/333497414
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PubChem-Substance/333497423
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PubChem-Substance/333497424
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PubChem-Substance/333497425
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PubChem-Substance/333497426
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PubChem-Substance/333497427
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PubChem-Substance/333497428
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PubChem-Substance/333497429
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PubChem-Substance/333497404
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PubChem-Substance/333497405
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PubChem-Substance/333497406
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PubChem-Substance/333497407
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PubChem-Substance/333497408
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PubChem-Substance/333497409
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PubChem-Substance/333497410
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PubChem-Substance/333497411
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PubChem-Substance/333497412
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PubChem-Substance/333497413
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PubChem-Substance/333497415
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PubChem-Substance/333497416
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PubChem-Substance/333497417
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PubChem-Substance/333497418
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PubChem-Substance/333497419
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PubChem-Substance/333497420
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PubChem-Substance/333497421
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PubChem-Substance/333497422