The C-32 Triacetyl-L-rhamnose Derivative of Ascomycin: A Potent, Orally Active Macrolactone Immunosuppressant

Journal of Medicinal Chemistry
1995.0

Abstract

Immunosuppressive drugs have been used for the prevention of organ transplant rejection and to some extent for the treatment of severe autoimmune disease for many years. Cyclosporin A (CsA) has dose-limiting liabilities including renal toxicity, hypertension, hirsutism, and tremors. Tacrolimus (FK-506), a more potent macrolactone immunosuppressant, has significant neurologic side effects. To develop a better-tolerated immunosuppressant, we targeted the macrocyclic lactone ascomycin (FK-520) and modified its C-32 hydroxyl group via glycosylation with triacetyl-L-rhamnose to obtain compound 1 (CP-123,369), a novel potent IL-2 biosynthesis inhibitor. The synthesis involved preparing triacetylglycosyl bromide from L-rhamnose, which was coupled to ascomycin using a silver-mediated glycosylation (17% overall yield, α anomer confirmed by NMR and X-ray crystallography). In vitro, compound 1 potently inhibits human T-lymphocyte proliferation (IC50 = 10.4 nM) and IL-2 production (IC50 = 11.0 nM), with potency similar to CsA and ~10-fold less than tacrolimus. In vivo, it showed oral activity in rat adjuvant arthritis (ED50: primary lesion 10.6 mg/kg, secondary lesion 2.3 mg/kg) and prevented rat heterotopic heart allograft rejection at 30 mg/kg. Importantly, 14-21 day rodent toxicology studies demonstrated compound 1 has a favorable therapeutic index (>10) relative to neurologic side effects (plasma drug concentration and dose), compared to tacrolimus (~2), with no toxicity at doses providing equal or greater immunosuppressive activity than tacrolimus.

Knowledge Graph

Similar Paper

The C-32 Triacetyl-L-rhamnose Derivative of Ascomycin: A Potent, Orally Active Macrolactone Immunosuppressant
Journal of Medicinal Chemistry 1995.0
Studies on an immunosuppressive macrolactam, ascomycin: Synthesis of a C-33 hydroxyl derivative
Bioorganic & Medicinal Chemistry Letters 1998.0
C32-O-imidazol-2-yl-methyl ether derivatives of the immunosuppressant ascomycin with improved therapeutic potential
Bioorganic & Medicinal Chemistry Letters 1998.0
Preparation and in vitro activity of aryl ether derivatives of the FK-506 related immunosuppressive macrolides ascomycin and L-683,742
Bioorganic & Medicinal Chemistry Letters 1995.0
32-Ascomycinyloxyacetic Acid Derived Immunosuppressants. Independence of Immunophilin Binding and Immunosuppressive Potency
Journal of Medicinal Chemistry 1998.0
Potent immunosuppressive C32-O-arylethyl ether derivatives of ascomycin with reduced toxicity
Bioorganic & Medicinal Chemistry Letters 1999.0
Preparation and immunosuppressive activity of 32-(O)-acylated and 32-(O)-thioacylated analogues of ascomycin
Bioorganic & Medicinal Chemistry Letters 1999.0
Synthesis and Biological Evaluation of Celastrol Derivatives as Potential Immunosuppressive Agents
Journal of Natural Products 2020.0
Alkyl ether derivatives of the FK-506 related, immunosuppressive macrolide L-683,742 (C31-O-desmethyl ascomycin)
Bioorganic & Medicinal Chemistry Letters 1994.0
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