Identification of new geldanamycin derivatives from unexplored microbial culture extracts using a MS/MS library

The Journal of Antibiotics
2017.0

Abstract

Natural microbial products are important resources for pharmaceuticals. Geldanamycin derivatives, as heat shock protein 90 (Hsp90) inhibitors, hold promise in cancer therapy. We developed a LC-MS-based dereplication method to identify geldanamycin derivatives from actinomycetes culture broths. Using a LTQ XL ion trap mass spectrometer, we investigated fragmentation patterns of geldanamycins under electrospray ionization (ESI) LC-MS, generated in silico fragmentation libraries with Mass Frontier software, and analyzed ~500 crude extracts from in-house-collected actinomycetes. A Streptomyces sp. W1348 strain was identified, producing five decarbamoyl 4,5-dihydrogeldanamycin derivatives (1–5). Compounds 1–3 were known, while 4 and 5 were new (compound 4 was unstable and spontaneously converted to 1 during purification). NMR analysis confirmed their decarbamoyl (C-7 free hydroxyl) and 4,5-dihydro (hydrogenated C-4/C-5 double bond) features, suggesting the strain lacks a functional carbamoyltransferase gene. New compound 5 (7-O-descarbamoyl-17-O-demethylreblastatin) provided insight into geldanamycin biosynthesis, revealing that C-17 hydroxylation precedes C-18/C-21 oxidation.

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