2,4-disubstituted triazine derivatives

Drug – bio-affecting and body treating compositions – Designated organic active ingredient containing – Heterocyclic carbon compounds containing a hetero ring...

Reexamination Certificate

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C544S194000, C544S208000, C544S209000, C544S213000

Reexamination Certificate

active

06638932

ABSTRACT:

The present invention is concerned with 2,4-disubstituted triazine derivatives having HIV replication inhibiting properties. The invention further relates to methods for their preparation and pharmaceutical compositions comprising them. The invention also relates to the use of said compounds in ihe manufacture of a medicament useful for the treatment of subjects suffering from HV (Human Immunodeficiency Virus) infection.
EP-0,834,507 discloses substituted diamino 1,3,5-triazine derivatives having HIV replication inhibiting properties. The present compounds differ from the known 1,3,5-triazines by structure and by their improved HIV replication inhibiting properties.
The present invention concerns the use of the compounds of formula
the N-oxides, pharmaceutically acceptable addition salts, quaternary amines and stereochemically isomeric forms thereof, wherein
—a
1
═a
2
—a
3
═a
4
— represents a bivalent radical of formula
—CH═CH—CH═CH—  (a-1);
—N═CH—CH═CH—  (a-2);
—N═CH—N═CH—  (a-3);
—N═CH—CH═N—  (a-4);
—N═N—CH═CH—  (a-5);
n is 0, 1, 2, 3 or 4; and in case —a
1
═a
2
—a
3
═a
4
— is (a-1), then n may also be 5;
R
1
is hydrogen, aryl, formyl, C
1-6
alkylcarbonyl, C
1-6
alkyl, C
1-6
alkyloxycarbonyl, C
1-6
alkyl substituted with formyl, C
1-6
alkylcarbonyl, C
1-6
alkyloxycarbonyl; and
each R
2
independently is hydroxy, halo, C
1-6
alkyl optionally substituted with cyano or —C(═O)R
4
, C
3-7
cycloalkyl, C
2-6
alkenyl optionally substituted with one or more halogen atoms or cyano, C
2-6
alkynyl optionally substituted with one or more halogen atoms or cyano, C
1-6
alkyloxy, C
1-6
alkyloxycarbonyl, carboxyl, cyano, nitro, amino, mono- or di(C
1-6
alkyl)amino, polyhalomethyl, polyhalomethyloxy, polyhalomethylthio, —S(═O)
p
R
4
, —NH—S(═O)R
4
, —C(═O)R
4
, —NHC(═O)H, —C(═O)NHNH
2
, —NHC(═O)R
4
, —C(═NH)R
4
or a radical of formula
wherein
each A independently is N, CH or CR
4
;
B is NH, O, S or NR
4
;
p is 1 or 2; and
R
4
is methyl, amino, mono- or dimethylamino or polyhalomethyl;
L is C
1-10
alkyl, C
2-10
alkenyl, C
2-10
alkynyl, C
3-7
cycloalkyl, whereby each of said aliphatic group may be substituted with one or two substituents independently selected from
C
3-7
cycloalkyl,
indolyl or isoindolyl, each optionally substituted with one, two, three or four substituents each independently selected from halo, C
1-6
alkyl, hydroxy, C
1-6
alkyloxy, cyano, aminocarbonyl, nitro, amino, polyhalomethyl, polyhalomethyloxy and C
1-6
alkylcarbonyl,
phenyl, pyridinyl, pyrimidinyl, pyrazinyl or pyridazinyl, wherein each of said aromatic rings may optionally be substituted with one, two, three, four or five substituents each independently selected from the substituents defined in R
2
; or
L is —X—R
3
wherein
R
3
is phenyl, pyridinyl, pyrimidinyl, pyrazinyl or pyridazinyl, wherein each of said aromatic rings may optionally be substituted with one, two, three, four or five substituents each independently selected from the substituents defined in R
2
; and
X is —NR
1
—, —NH—NH—, —N═N—, —O—, —C(═O)—, —CHOH—, —S—, —S(═O)— or —S(═O)
2
—;
aryl is phenyl or phenyl substituted with one, two, three, four or five substituents each independently selected from halo, C
1-6
alkyl, C
3-7
cycloalkyl, C
1-6
alkyloxy, cyano, nitro, polyhaloC
1-6
alkyl and polyhaloC
1-6
alkyloxy;
for the manufacture of a medicine for the treatment of subjects suffering from HIV (Human Immunodeficiency Virus) infection.
This invention also concerns compounds of formula (I′) which are defined as compounds of formula (I) wherein the compounds cited in the following references
Recl. Trav. Chim. Pays-Bas (1969), 88(4), 426-38.
Polym. J. (Tokyo) (1996), 28(4), 337-42.
J. Inst. Chem. (India) (1978), 50(5), 213-14.
Nippon Kagaku Kaishi (1977), Issue 4, 549-55.
Kobunshi Kagaku (1973), 30(12), 720-6.
SU 189438
DE 2226474
are excluded;
i.e. compounds of formula
the N-oxides, addition salts, quaternary amines and stereochemically isomeric forms thereof, wherein the substituents are as defined under formula (I); with the proviso that compounds wherein
L is C
1-3
alkyl; R
1
is selected from hydrogen, ethyl and methyl; —a
1
═a
2
—a
3
═a
4
— represents a bivalent radical of formula (a-1); n is 0 or 1 and R
2
is selected from fluoro, chloro, methyl, trifluoromethyl, ethyloxy and nitro; or
L is —X—R
3
, X is —NH—; R
1
is hydrogen; —a
1
═a
2
—a
3
═a
4
— represents a bivalent radical of formula (a-1); n is 0 or 1 and R
2
is selected from chloro, methyl, methyloxy, cyano, amino and nitro and R
3
is phenyl, optionally substituted with one substituent selected from chloro, methyl, methyloxy, cyano, amino and nitro;
and the compounds
N,N′-dipyridinyl-(1,3,5)-triazine-2,4-diamine;
(4-chloro-phenyl)-(4(1-(4-isobutyl-phenyl)-ethyl)-(1,3,5) triazin-2-yl)-amine
are not included.
A special group of compounds are compounds of formula (I′), the N-oxides, addition salts, quaternary amines and stereochemically isomeric forms thereof, wherein
—a
1
═a
2
—a
3
═a
4
— represents a bivalent radical of formula
—CH═CH—CH═CH—  (a-1);
—N═CH—CH═CH—  (a-2);
—N═CH—N═CH—  (a-3);
—N═CH—CH═N—  (a-4);
—N═N—CH═CH—  (a-5);
n is 0, 1, 2, 3 or 4; and in case —a
1
═a
2
—a
3
═a
4
— is (a-1), then n may also be 5;
R
1
is hydrogen, aryl, formyl, C
1-6
alkylcarbonyl, C
1-6
alkyl, C
1-6
alkyloxycarbonyl, C
1-6
alkyl substituted with formyl, C
1-6
alkylcarbonyl, C
1-6
alkyloxycarbonyl; and
each R
2
independently is hydroxy, halo, C
1-6
alkyl optionally substituted with cyano or —C(═O)R
4
, C
3-7
cycloalkyl, C
2-6
alkenyl optionally substituted with one or more halogen atoms or cyano, C
2-6
alkynyl optionally substituted with one or more halogen atoms or cyano, C
1-6
alkyloxy, C
1-6
alkyloxycarbonyl, carboxyl, cyano, nitro, amino, mono- or di(C
1-6
alkyl)amino, polyhalomethyl, polyhalomethyloxy, polyhalomethylthio, —S(═O)
p
R
4
, —NH—S(═O)
p
R
4
, —C(═O)R
4
, —NHC(═O)H, —C(═O)NHNH
2
, —NHC(═O)R
4
, —C(═NH)R
4
or a radical of formula
wherein
each A independently is N, CH or CR
4
;
B is NH, O, S or NR
4
;
p is 1 or 2; and
R
4
is methyl, amino, mono- or dimethylamino or polyhalomethyl;
L is C
4-10
alkyl, C
2-10
alkenyl, C
2-10
alkynyl, C
3-7
cycloalkyl, whereby each of said aliphatic group may be substituted with one or two substituents independently selected from
C
3-7
cycloalkyl,
indolyl or isoindolyl, each optionally substituted with one, two, three or four substituents each independently selected from halo, C
1-6
alkyl, hydroxy, C
1-6
alkyloxy, cyano, aminocarbonyl, nitro, amino, polyhalomethyl, polyhalomethyloxy and C
1-6
alkylcarbonyl,
phenyl, pyridinyl, pyrimidinyl, pyrazinyl or pyridazinyl, wherein each of said aromatic rings may optionally be substituted with one, two, three, four or five substituents each independently selected from the substituents defined in R
2
; or
L is —X—R
3
wherein
R
3
is phenyl, pyridinyl, pyrimidinyl, pyrazinyl or pyridazinyl, wherein each of said aromatic rings may optionally be substituted with two, three, four or five substituents each independently selected from the substituents defined in R
2
; and
X is —NR
1
—, —NH—NH—, —N═N—, —O—, —C(═O)—, —CHOH—, —S—, —S(═O)— or —S(═O)
2
—;
aryl is phenyl or phenyl substituted with one, two, three, four or five substituents each independently selected from halo, C
1-6
alkyl, C
3-7
cycloalkyl, C
1-6
alkyloxy, cyano, nitro, polyhaloC
1-6
alkyl and polyhaloC
1-6
alkyloxy;
and suitably N,N′-dipyridinyl-(1,3,5)-triazine-2,4-diamine is excluded.
Another special group of compounds are those compounds having the formula
the N-oxides, addition salts, quaternary amines and stereochemically isomeric forms thereof, wherein
—b
1
═b
2
—C(R
2a
)═b
3
—b
4
═ represents a bivalent radical of formula
—CH═CH—C

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