Chemical phylogenetics of histone deacetylases

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Abstract
In contrast to perceived nonselectivity, biochemical profiling reveals that currently available HDAC inhibitors predominantly inhibit only class I and IIb HDAC enzymes. A new pan-selective inhibitor, obtained by screening a focused library, provides an important tool for studying class IIa HDACs. The broad study of histone deacetylases in chemistry, biology and medicine relies on tool compounds to derive mechanistic insights. A phylogenetic analysis of class I and II histone deacetylases (HDACs) as targets of a comprehensive, structurally diverse panel of inhibitors revealed unexpected isoform selectivity even among compounds widely perceived as nonselective. The synthesis and study of a focused library of cinnamic hydroxamates allowed the identification of, to our knowledge, the first nonselective HDAC inhibitor. These data will guide a more informed use of HDAC inhibitors as chemical probes and therapeutic agents.