Pyrimidine bisphosphonate esters and (alkoxymethylphosphinyl)alk

Drug – bio-affecting and body treating compositions – Designated organic active ingredient containing – Phosphorus containing other than solely as part of an...

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544117, 544122, 544123, 544232, 544243, 544244, 514 86, A61K 31675, C07F 96512, C07F 96561

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056354959

DESCRIPTION:

BRIEF SUMMARY
BACKGROUND OF THE INVENTION

The present invention is directed toward pyrazolopyrimidine (Formula 1) and pyrimidinyl (Formula 2) (alkoxymethylphosphinyl)alkyl phosphonic acids, pyrimidine bisphosphonates (Formula 3) and their pharmaceutically acceptable salts which are useful as anti-inflammatories, anti-arthritic agents and in the case of Formula 3, Ca-channel blockers useful in cardiovascular diseases.
The subject compounds are also useful for treating arthritis and its related symptoms such as inflammation and prevention of excessive bone regrowth and remodeling while showing a decreased bone affinity. One class of such compounds which still maintain anti-resorptive activity are the phosphinyl-phosphonic acids prepared by Ebitino et al., cited below.


DESCRIPTION OF THE RELATED ART

The following related art are bisphosphonic tetraester or acids directed toward Formulas 1 and 2:
U.S. Pat. No. 4,746,654 discloses bisphosphonates useful as anti-inflammatory agents, Australian Patent A-51534/85 discloses bisphosphonates useful in treating abnormal calcium and phosphorous metabolism and useful in treating arthritis.
U.S. Pat. No. 3,683,080 discloses polyphosphonates, in particular diphosphonates useful in inhibiting anomalous deposition and mobilization of calcium phosphate in animal tissue.
DE 3,719,513-A (Derwent 89-000580/01) discloses diphosphonic acid derivatives useful in treatment of disorders of calcium metabolism.
With respect to Formula 1 compounds, the alkylation of 5,7-dimethyl pyrazolo[1,5-a]pyrimidines was disclosed at the American Chemical Society spring meeting on Jun. 9, 1988, PD 7244-88-021.
Yamanouchi has published imidazo[1,2-a]pyridines and imidazo[1,2-a]imidazoles (EP 354-806 A2, Feb. 14, 1990). Boehringer Mannheim DE 3626-058 A1 discloses heteroaromatic diphosphonates bound to a diphosphonate.
The following related an disclose bisphosphonic tri-esters or acid with an alkyl substituent:
Savignac, et al., Carbanions Phosphonates, J. of Organometallic Chem., 312:283-95 (1986); and
Ebetino, F. H., "Phosphate Containing Bone Active Heterocycles," Heterocycles 30(2):855-62 (1990).
The following related art are directed toward compounds of Formula 3:
AU-A-5153485 (publication date Jun. 26, 1986) (EP 186 405) discloses pyrimidine bisphosphonates related to the compounds of the present invention. The substituents on the pyrimidine ring, however, are hydrogen, methyl, amino, methoxy, nitro, hydroxy, and combinations thereof; whereas, the subject invention precludes these substituents in favor of the X.sup.1 group as defined below.
U.S. Pat. No. 4,696,920 discloses 1,3 diphosphonates useful for the treatment of cardiovascular diseases.


SUMMARY OF THE INVENTION

In one aspect, the subject invention consists of pyrazolopyrimidine (Formula 1) and pyrimidinyl (Formula 2) (alkoxymethylphosphinyl)alkyl phosphonic esters, acids and their pharmaceutically acceptable salts, which are structurally represented as: ##STR2## wherein X is O or S; each R.sub.1 is the same or different and is selected from the group consisting of H, Na, K, tromethamine, C.sub.1 -C.sub.6 alkyl, CH.sub.2 -phenyl, phenyl (optionally substituted with 1 to 5 NO.sub.2, halo, or C.sub.1 -C.sub.4 alkyl), or both R.sub.1 's on the same phosphorus atom are taken together to be --CH.sub.2 --CH.sub.2 --, --CH.sub.2 --CH.sub.2 --CH.sub.2 --, or --CH.sub.2 --C(CH.sub.3).sub.2 --CH.sub.2 -- whereby a heterocyclic ring is formed; -C.sub.6 alkoxy, phenoxy, C.sub.3 -C.sub.7 cycloalkyl, phenyl (optionally substituted with 1 or 2 phenyls, or 1 to 5 halo, NO.sub.2, CN, CF.sub.3, C.sub.1 -C.sub.10 alkyl, C.sub.3 -C.sub.7 cycloalkyl, C.sub.1 -C.sub.6 alkoxy or C.sub.1 -C.sub.6 alkylthio), 2-, 4- or 5-pyrimidyl (optionally substituted with 1 or 2 phenyls, or 1 to 3 halo, NO.sub.2, CN, CF.sub.3, C.sub.1 -C.sub.10 alkyl, C.sub.3 -C.sub.7 cycloalkyl, C.sub.1 -C.sub.6 alkoxy, or C.sub.1 -C.sub.6 alkylthio), 2-, 3- or 4-pyridyl (optionally substituted with 1 or 2 phenyls, or 1 to 4 halo, NO.sub.2, CN, CF.sub.3, C.sub.1 -C.sub.10 alkyl, C.sub.3 -C.sub.7

REFERENCES:
patent: 3683080 (1972-08-01), Francis
patent: 4696920 (1987-09-01), Bentzen et al.
patent: 4746654 (1988-05-01), Breliere et al.
patent: 5397774 (1995-03-01), Nugent et al.
Alkylation of 5,7-dimethyl pyrazolo[1,5-a]pyrimidines, American Chemical Society Spring meeting (Jun. 8, 1988), PD 7244-88-021.
Ebetino, F.H. et al., "Recent Work on the Synthesis of Phosphonate-Containing, Bone-Active Heterocycles", Heterocycles 30(2):855-62 (1990).
Teulade, M-P and P. Savignac, "Carbanions Phosphonates .alpha.-Lithies: Synthese, Basicite Comparee, et Stabilitea L'Autocondensation," J. of Organometalic Chem. 312:283-95 (1986).
Gompper, Chemical Abstracts vol. 54, No. 9955b (1960).
Gompper, Chem. Ber. vol. 93, pp. 198-209 (1960).
Abstract for DE 3719513 (Dec. 22, 1988).
Abstract for DE 3,626,058 (Feb. 11, 1988).

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