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CAS No. : | 492431-11-5 | MDL No. : | MFCD05864738 |
Formula : | C13H19ClN4O2 | Boiling Point : | - |
Linear Structure Formula : | - | InChI Key : | MIXODQAAOQHDTG-UHFFFAOYSA-N |
M.W : | 298.77 | Pubchem ID : | 21925370 |
Synonyms : |
|
Signal Word: | Warning | Class: | N/A |
Precautionary Statements: | P261-P305+P351+P338 | UN#: | N/A |
Hazard Statements: | H302-H315-H319-H335 | Packing Group: | N/A |
GHS Pictogram: |
* All experimental methods are cited from the reference, please refer to the original source for details. We do not guarantee the accuracy of the content in the reference.
Yield | Reaction Conditions | Operation in experiment |
---|---|---|
With caesium carbonate; In N,N-dimethyl-formamide; at 120℃; for 2.0h;Microwave irradiation; | EXAMPLE 92; 5,5-Dimethyl-2-(6-[r6-piperazin-l-ylpyridazin-3-yl)oxy]-2,3-dihydro-4H-L4- benzoxazin-4-vU -5.6-dihydro- 1 ,3 -benzothiazol-7(4/f)-one; A mixture of 3,6-dichloropyridazine (0.60 g, 3.24 mmol), l-5(9C-piperazine (0.48 g, 3.24 mmol) and DIPEA (0.60 tnL, 3.24 mmol) in THF (20 mL) was heated to 14O0C under microwave irradiation for 3h. After cooling to r.t. it was concentrated in vacuo and purified by column chromatography (SiO2, 0-50% EtOAc in heptane) to give a white solid. A mixture of this material (crude pyridazinyl piperazine, 45 mg, 0.15 mmol),Example 6 (50 mg, 0.15 mmol) and cesium carbonate (98 mg, 0.3 mmol) in DMF (4 mL) was heated to 12O0C under microwave irradiation for 2h. After cooling to r.t. the mixture was concentrated in vacuo and purified by prep HPLC to give an off-white solid (26 mg, 30%). deltaH (CDCl3) 1.13 (6H, s), 1.48 (9H, s), 2.41 (2H, s), 2.74 (2H, s), 3.14 (8H, br.s), 4.15-4.24 (2H, m), 4.30-4.38 (2H5 m), 6.89-7.00 (2H, m), 7.26 (2H, s), 7.89 (IH, d, J 2.4 Hz). LCMS (ES+) 593 (M+H)+. |
Yield | Reaction Conditions | Operation in experiment |
---|---|---|
88% | With N-ethyl-N,N-diisopropylamine; In 1,4-dioxane; at 80℃; | Synthesis of tert-butyl 4-(6-chloropyridazin-3-yl)piperazine-1-carboxylate To a solution of 3,6-dichloropyridazine (Sigma-Aldrich, St. Louis, Mo.) (57.3 g, 385 mmol) in 1,4-dioxane (250 mL) were added tert-butyl piperazine-1-carboxylate (Sigma-Aldrich) (71.6 g, 358 mmol) and N,N-diisopropylethylamine (66.9 mL, 385 mmol). The mixture was stirred overnight at 80 C. then concentrated under reduced pressure. The residue was dissolved in ethyl acetate (3 L) and washed with 10% citric acid, water, and brine. The organic layer was concentrated and the residue was re-crystallized in ethyl acetate to provide tert-butyl 4-(6-chloropyridazin-3-yl)piperazine-1-carboxylate as an off-white solid (101 g, 88% yield). 1H NMR (400 MHz, CDCl3) delta ppm 1.25 (9H, s), 3.26-3.47 (8H, m), 6.67 (1H, d, J=9.6 Hz), 7.00 (1H, d, J=9.6 Hz); MS (ESI) m/z: 299.0 [M+H]+. |
70% | With triethylamine; In N,N-dimethyl-formamide; at 80℃; | A solution of 3,6-dichloropyridazine (5.01 g, 33.6 mmol) and tert-butyl piperazine-1-carboxylate (6.88g, 37.0 mmol) in DMF (50 mL) was added triethylamine (11.7 mL, 50.4 mmol) and stirred at 80C overnight. The resultant reaction mixture was cooled to room temperature, and water was added to the mixture. The mixture was extracted three times with a solvent mixture of dichloromethane and methanol (95:5) (50 mL). The resultant organic phases were combined together and dried over anhydrous magnesium sulfate. The resultant solid was separated by filtration, and the filtrate was then concentrated under reduced pressure. The resultant crude product was washed with diethyl ether to yield the title compound (7.0 g, 70%). |
70% | With triethylamine; In N,N-dimethyl-formamide; at 80℃; | 3,6-Dichloropyridazine (5.01 g, 33.6 mmol) and tert-butyl piperazine-1-carboxylate (6.88 g, 37.0 mmol) were dissolved in DMF (50 mL). Triethylamine (11.7 mL, 50.4 mmol) was added to the solution. The resulting mixture was stirred at 80C overnight. The reaction mixture was cooled to room temperature and water was added. The solution was extracted with a 95:5 mixed solvent (50 mL) of dichloromethane and methanol three times. The combined organic phase was dried over anhydrous magnesium sulfate. The solid was filtered out, and the filtrate was concentrated under reduced pressure. The crude product was washed with diethyl ether to give the title compound (7.0 g, yield: 70%). |
63% | With triethylamine; In toluene; at 110℃; for 16.0h; | Preparation of tert-Butyl 4-(6-chloropyridazin-3-yl)piperazine-1-carboxylate 6-3: (1202) (1203) A stirred mixture of 3,6-dichloropyridazine 6-1 (2.0 g, 13.4 mmol), tert-butyl piperazine- 1-carboxylate 6-2 (3.72 g, 20.0 mmol) and triethylamine (2.78 mL, 20.0 mmol) in toluene (20mL) was heated at 110 C for 16 h. After complete consumption of 6-1 as evident from TLC, the volatiles were stripped off, residue partitioned between ethyl acetate and water, combined organic extracts evaporated to afford a crude residue which was purified column chromatography (elution with 30% ethyl acetate/Hexane) to afford tert-butyl 4-(6-chloropyridazin-3- yl)piperazine-1-carboxylate 6-3 (2.52 g, 8.46 mmol, 63.0 %) as an off-white solid. LC MS: ES+ 299.2 |
With triethylamine; In butan-1-ol; for 5.0h;Heating / reflux; | A mixture of 13.52 g of tert-butyl 1-piperazinecarboxylate, 10.81 g of 3,6-dichloropyridazine and 20 ml of triethylamine in 100 ml of n-butanol is heated at reflux for 5 hours. It is concentrated under vacuum and the residue is chromatographed on silica gel, eluting with a DCM/AcOEt (90/10; v/v) mixture. This gives 14 g of the expected product, which is used as it is. | |
With N-ethyl-N,N-diisopropylamine; In tetrahydrofuran; at 140℃; for 3.0h;Microwave irradiation; | EXAMPLE 92; 5,5-Dimethyl-2-(6-[r6-piperazin-l-ylpyridazin-3-yl)oxy]-2,3-dihydro-4H-L4- benzoxazin-4-vU -5.6-dihydro- 1 ,3 -benzothiazol-7(4/f)-one; A mixture of 3,6-dichloropyridazine (0.60 g, 3.24 mmol), l-5(9C-piperazine (0.48 g, 3.24 mmol) and DIPEA (0.60 tnL, 3.24 mmol) in THF (20 mL) was heated to 14O0C under microwave irradiation for 3h. After cooling to r.t. it was concentrated in vacuo and purified by column chromatography (SiO2, 0-50% EtOAc in heptane) to give a white solid. A mixture of this material (crude pyridazinyl piperazine, 45 mg, 0.15 mmol),Example 6 (50 mg, 0.15 mmol) and cesium carbonate (98 mg, 0.3 mmol) in DMF (4 mL) was heated to 12O0C under microwave irradiation for 2h. After cooling to r.t. the mixture was concentrated in vacuo and purified by prep HPLC to give an off-white solid (26 mg, 30%). deltaH (CDCl3) 1.13 (6H, s), 1.48 (9H, s), 2.41 (2H, s), 2.74 (2H, s), 3.14 (8H, br.s), 4.15-4.24 (2H, m), 4.30-4.38 (2H5 m), 6.89-7.00 (2H, m), 7.26 (2H, s), 7.89 (IH, d, J 2.4 Hz). LCMS (ES+) 593 (M+H)+. | |
With triethylamine; In butan-1-ol; for 5.0h;Heating / reflux; | A mixture of 13.52 g of tert-butyl 1-piperazinecarboxylate, 10.81 g of 3,6-dichloro-pyridazine and 20 ml of triethylamine in 100 ml of n-butanol is refluxed for 5 hours. The mixture is concentrated under vacuum and the residue is chromatographed on silica gel, eluting with a DCM/EtOAc mixture (90/10; v/v). 14 g of the expected product are obtained, and are used without further purification. | |
With N-ethyl-N,N-diisopropylamine; In tert-butyl alcohol; at 100 - 150℃; for 0.833333h;Microwave irradiation; | Intermediate 141 ,1 -dimethylethyl 4-(6-chloro-3-pyridazinyl)-1 -piperazinecarboxylate In a microwave vial were mixed: 1 ,1 -dimethylethyl 1 -piperazinecarboxylate(135 mg, 0.725 mmol, available from Fluka), 3,6-dichloropyridazine (90 mg, 0.604 mmol, available from Alfa Aesar) and DIPEA (0.137 mL, 0.785 mmol) in Tert-Butanol (2 mL). The reaction was stirred and heated in an Emrys Optimizer microwave at 100C for 20 mins then for 30 mins at 150C. The reaction mixture was partitioned between EtOAc (20mL) and water (20mL) and the organic layer washed with brine (20mL) before being dried through an hydrophobic frit and concentrated. The residue was dissolved in DCM and purified by SP4 on a 12+M silica cartridge using a gradient of 10-50% EtOAc in cyclohexane. The appropriate fractions were collected and concentrated to yield the desired product as a white solid, 1 ,1 -dimethylethyl 4-(6-chloro-3-pyridazinyl)-1 - piperazinecarboxylate (1 14.2 mg). LCMS (Method C): Rt = 0.85, MH+ = 299 | |
With N-ethyl-N,N-diisopropylamine; In tert-butyl alcohol; at 100 - 150℃; for 0.833333h;Microwave irradiation; | In a microwave vial were mixed: 1,1-dimethylethyl 1-piperazinecarboxylate (135 mg, 0.725 mmol, available from Fluke), 3,6-dichloropyridazine (90 mg, 0.604 mmol, available from Alfa Aesar) and DIPEA (0.137 mL, 0.785 mmol) in Tert-Butanol (2 mL). The reaction was stirred and heated in an Emrys Optimizer microwave at 100 C. for 20 mins then for 30 mins at 150 C. The reaction mixture was partitioned between EtOAc (20 mL) and water (20 mL) and the organic layer washed with brine (20 mL) before being dried through an hydrophobic frit and concentrated. The residue was dissolved in DCM and purified by SP4 on a 12+M silica cartridge using a gradient of 10-50% EtOAc in cyclohexane. The appropriate fractions were collected and concentrated to yield the desired product as a white solid, 1,1-dimethylethyl 4-(6-chloro-3-pyridazinyl)-1-piperazinecarboxylate (114.2 mg). LCMS (Method C): Rt=0.85, MH+=299 |
Yield | Reaction Conditions | Operation in experiment |
---|---|---|
With hydrogen;palladium 10% on activated carbon; In DMF (N,N-dimethyl-formamide); ethanol; at 20℃; under 760.051 Torr; | A mixture of 10.5 g of the compound obtained in the preceding step and 2.5 g of 10% palladium on carbon in 30 ml of DMF and 250 ml of EtOH is hydrogenated at AT under atmospheric pressure overnight. The catalyst is filtered off and the filtrate is concentrated under vacuum. The residue is chromatographed on silica gel, eluting with a DCM/MeOH (97/3 to 90/10; v/v) mixture. This gives 9.1 g of the expected product, which is used as it is. | |
With hydrogen;palladium 10% on activated carbon; In DMF (N,N-dimethyl-formamide); ethanol; at 20℃; under 760.051 Torr; | A mixture of 10.5 g of the compound obtained in the preceding step and 2.5 g of 10% palladium-on-charcoal in 30 ml of DMF and 250 ml of EtOH is hydrogenated overnight at RT and atmospheric pressure. The catalyst is filtered off and the filtrate is concentrated under vacuum. The residue is chromatographed on silica gel, eluting with a DCM/MeOH mixture of from (97/3; v/v) to (90/10; v/v). 9.1 g of the expected product are obtained, and are used without further purification. |
Yield | Reaction Conditions | Operation in experiment |
---|---|---|
With hydrogenchloride; In methanol; at 20℃; | A mixture of 2.96 g of the compound obtained in step A of preparation 3.3 and 30 ml of a 6N solution of HCl in MeOH is left with stirring in AT overnight. The reaction mixture is concentrated under vacuum, the residue is taken up in DCM a number of times and each time the solvent is evaporated under vacuum. This gives 2.6 g of the expected product, which is used as it is. |
Yield | Reaction Conditions | Operation in experiment |
---|---|---|
With trifluoroacetic acid; In dichloromethane; at 20℃; for 0.75h; | A. To an ice cold solution of 4-(6-chloropyridazin-3-yl)piperazine-1- carboxylic acid tert-butyl ester (2.00 g, 6.69 mmol) in dichloromethane (10 mL) was carefully added trifluoroacetic acid (2 mL). The mixture was stirred for 45 minutes at room temperature and then concentrated in vacuo to afford the crude 3-chloro-6- piperazin-1-ylpyridazine (~1.0 g) which was used in the next reaction without further purification. MS (ES+) m/z 199.1 (M+1 ). |
Yield | Reaction Conditions | Operation in experiment |
---|---|---|
With sodium t-butanolate;tris-(dibenzylideneacetone)dipalladium(0); 4,5-bis(diphenylphos4,5-bis(diphenylphosphino)-9,9-dimethylxanthenephino)-9,9-dimethylxanthene; In 1,4-dioxane; at 120℃; for 6.0h; | A mixture of tert-butyl 4- (6-chloropyridazin-3-yl)piperazine-l-carboxylate (0.060 g, 0.20 mmol), compound 83 (0.054 g, 0.20 mmol), Xantphos (0.017 g, 0.030 mmol), Pd2(dba)3 (0.014 g, 0.015 mmol), and sodium tert-butoxide (0.029 g, 0.30 mmol) in dioxane was purged with nitrogen gas for 1 minute. The reaction was heated at 12O0C for 6 hours and then cooled to room temperature. The solvent was removed by filtration. The residue was washed with 2 x ImI dioxane. The product was then dissolved in 1OmL methanol/DCM (1 :1) and concentrated. The crude material was re-dissolved in 4mL methanol and purified on a C-18 reversephase column (150 x 30 mm, 4 micro) using Mass directed preperative HPLC and gradient elution of acetonitrile in water containing 0.1%TFA to give the title compound 162. LCMS-ESI (POS), M/Z, M+l: 532.3 |
Yield | Reaction Conditions | Operation in experiment |
---|---|---|
76% | With tris-(dibenzylideneacetone)dipalladium(0); caesium carbonate; 2,2'-bis-(diphenylphosphino)-1,1'-binaphthyl; In toluene; at 100℃; | Tert-butyl 4-(6-chloropyridazin-3-yl)piperazine-1-carboxylate synthesized in Reference Example 17 (59.8 mg, 0.20 mmol, benzophenone imine (43.5 mg, 0.24 mmol), tris(dibenzylideneacetone)dipalladium (9.2 mg, 0.010 mmol), BINAP (12.5 mg, 0.020 mmol), and cesium carbonate (130.3 mg, 0.40 mmol) were suspended in toluene (1.0 mL), and the suspension was stirred at 100C overnight. The resultant reaction mixture was cooled to room temperature and then filtered through Celite, and the Celite was washed with ethyl acetate. The filtrate was washed with saturated brine and dried over anhydrous magnesium sulfate, and the solid was separated by filtration. The filtrate was concentrated under reduced pressure, and the residue was purified by silica gel column chromatography to yield the title compound (67 mg, 76%). |
76% | With tris-(dibenzylideneacetone)dipalladium(0); caesium carbonate; 2,2'-bis-(diphenylphosphino)-1,1'-binaphthyl; In toluene; at 100℃; | The <strong>[492431-11-5]tert-butyl 4-(6-chloropyridazin-3-yl)piperazine-1-carboxylate</strong> (59.8 mg, 0.20 mmol) prepared in Referential Example 14, benzophenone imine (43.5 mg, 0.24 mmol), tris(dibenzylideneacetone)dipalladium (9.2 mg, 0.010 mmol), BINAP (12.5 mg, 0.020 mmol) and cesium carbonate (130.3 mg, 0.40 mmol) were suspended in toluene (1.0 mL). The reaction mixture was stirred at 100C overnight. The reaction mixture was cooled to room temperature and filtered through a Celite pad. The Celite pad was washed with ethyl acetate. The filtrate was washed with saturated brine, and dried over anhydrous magnesium sulfate. The solid was filtered out, and the filtrate was concentrated under reduced pressure. The residue was purified by silica gel column chromatography to give the title compound (67 mg, yield: 76%). |
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