Microbial transformations of immunosuppressive compounds. IV. Hydroxylation and hemiketal formation of ascomycin(immunomycin) by Streptomyces sp. MA6970(ATCC No.55281).

The Journal of Antibiotics
1994.0

Abstract

The important immunosuppressive agents FK 506 and ascomycin (1) have been the focus of intensive structure-activity relationship (SAR) studies, with FK 506 recently approved by the FDA for liver organ transplantation in the U.S. Due to the complexity of their structures, we initiated a microbial transformation program to modify chemically inaccessible sites. Previously, we reported microbial desmethylation, specific methylation, and glucosylation of FK 506/ascomycin to obtain various derivatives that are difficult or tedious to synthesize chemically. In this study, we describe the specific hydroxylation of the 19-methyl group of ascomycin by Streptomyces sp. MA 6870 (ATCC No. 55281), leading to a novel hemiketal structure (2). The structure of 2 was characterized using FAB mass spectrometry (showing an M+Li ion of 814, consistent with a hydroxylated derivative) and 1H/13C NMR (revealing the absence of the H-19 methyl signal, loss of the C-22 carbonyl signal, and appearance of signals corresponding to a hemiketal carbon and hydroxylated C-19). The immunosuppressive activity of 2 was evaluated in an in vitro T cell proliferation assay, yielding an IC50 of 3 nM (compared to 0.8 nM for parent compound 1) and retaining 35% of the biological activity of 1.

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