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Li, Kaixuan ; Wang, Mingqian ; Akoglu, Melike , et al. ACS Pharmacol. Transl. Sci.,2023,6(3):410-421. DOI: 10.1021/acsptsci.2c00215 PubMed ID: 36926452
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Abstract: Bruton′s tyrosine kinase (BTK) is a target for treating B-cell malignancies and autoimmune diseases. To aid in the discovery and development of BTK inhibitors and improve clin. diagnoses, we have developed a positron emission tomog. (PET) radiotracer based on a selective BTK inhibitor, remibrutinib. [18F]PTBTK3 is an aromatic, 18F-labeled tracer that was synthesized in 3 steps with a 14.8 ± 2.4% decay-corrected radiochem. yield and ≥99% radiochem. purity. The cellular uptake of [18F]PTBTK3 was blocked up to 97% in JeKo-1 cells using remibrutinib or non-radioactive PTBTK3. [18F]PTBTK3 exhibited renal and hepatobiliary clearance in NOD SCID (non-obese diabetic/ severe combined immunodeficiency) mice, and the tumor uptake of [18F]PTBTK3 in BTK-pos. JeKo-1 xenografts (1.23 ± 0.30% ID/cc) was significantly greater at 60 min post injection compared to the tumor uptake in BTK-neg. U87MG xenografts (0.41 ± 0.11% ID/cc). In the JeKo-1 xenografts, tumor uptake was blocked up to 62% by remibrutinib, indicating the BTK-dependent uptake of [18F]PTBTK3 in tumors.
Keywords: PET imaging ; BTK ; tumor ; fluorine-18 ; Jeko-1 ; U87MG
Purchased from AmBeed: 38953-42-3 ; 57561-39-4 ; 158580-57-5 ; 1247927-81-6 ; 909698-09-5 ; 864262-97-5
CAS No. : | 158580-57-5 | MDL No. : | MFCD10699645 |
Formula : | C8H6BrNO4 | Boiling Point : | No data available |
Linear Structure Formula : | - | InChI Key : | YTWDMAAPIWOIFZ-UHFFFAOYSA-N |
M.W : | 260.04 | Pubchem ID : | 18350461 |
Synonyms : |
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Signal Word: | Warning | Class: | |
Precautionary Statements: | P261-P305+P351+P338 | UN#: | |
Hazard Statements: | H315-H319-H335 | Packing Group: | |
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 |
---|---|---|
96% | With tin(II) chloride dihdyrate; In ethyl acetate; at 30℃; for 2h;Ultrasonic irradiation; | Example 281 : 2-(3-Chlorobenzo[b1thiophene-2-carboxarnido)-4-(5-(4-chlorophenyl)-2- oxo-oxazolidin-3-yl)benzoic acidMethod 36SnCI2 x 2H20 (5 g, 22 mmol) was added to a solution of <strong>[158580-57-5]methyl 4-bromo-2-nitrobenzoate</strong> (0.6 g, 2.3 mmol) in ethyl acetate (20 ml). The reaction mixture was submitted to ultrasonic irradiation for 2 h at 30C until the reaction was complete as indicated by TLC analysis. The solvent was removed under reduced pressure and the crude residue was washed with 2 M KOH. The aqueous layer was extracted with further portions of ethyl acetate, and the combined organic extracts were washed with brine and water, dried (MgS04) and concentrated under reduced pressure. The crude residue waschromatographed over silica gel (ethyl acetate / hexanes) yielding methyl 4-bromo-2- aminobenzoate (96%).A solution of this compound (0.46 g, 2 mmol), 5-(4-chlorophenyl)oxazolidin-2-one (0.4 g, 2 mmol), Xantphos (128 mg, 0.22 mmol), Pd2(dba)3 (92 mg, 0.11 mmol) and K3P04 (2.2 mmol) in dioxane was refluxed for 7 h. After cooling, the solvent was evaporated under vacuum and the residue partitioned between water and ethyl acetate. The aqueous layer was extracted with further portions of ethyl acetate and the combined organic extracts were washed with brine and water, dried (MgS04) and concentrated under reduced pressure. The crude residue was chromatographed over silica gel (ethyl acetate / hexanes) yielding methyl 2-amino-4-(5-(4-chlorophenyl)-2-oxo-oxazolidin-3-yl)benzoate (71 %).This compound (0.35 g, 1 mmol) was dissolved in THF, and 1.1 mmol of 3-chloro- benzo[b]thiophene carbonyl chloride was added. The reaction mixture was refluxed for 14 h and concentrated under vacuum. The crude reaction mass was washed with diethyl ether two times and dissolved in THF-water (3: 1). LiOH (1.1 mmol) was added and the solution was stirred overnight at room temperature, concentrated under vacuum, and the residue was dissolved in the minimum volume of water. After adjusting the pH to 6-7, the aqueous solution was extracted with ethyl acetate. The organic layer was dried (MgS04) and concentrated under vacuum to afford the title compound (50%), mp >200C.1 H NMR (400 MHz, DMSO-cfe) delta ppm: 13.70 (br.s, 1 H), 12.40 (br.s, 1 H), 8.93 (s, 1 H), 8.18 (m, 1 H), 8.09 (d, 1 H), 7.98 (m, 1 H), 7.64 (m, 2H), 7.59 (m, 2H), 7.53 (m, 3H), 5.83 (m, 1 H), 4.57 (m, 1 H), 4.04 (m, 1 H); MS: m/z = 527 [MH]+ |
96% | With hydrogen;5%-palladium/activated carbon; In methanol; under 2585.81 Torr; for 1h; | 4-Bromo-2-aminomethylbenzoate : [00190] 4-Bromo-2-nitromethylbenzoate (300MG ; 1. 15MMOL) was dissolved in 25ML of methanol and shaken with 5% Pd (c) under hydrogen atmosphere (50 PSI) for 1 hour. The reaction was filtered through celite and evaporated to give the product as a white solid (255mg; 96%). MS: MH+= 230 |
93% | With tin(ll) chloride; In dichloromethane; ethyl acetate; at 20℃; | A. Methyl 2-amino-4-bromobenzoate To a stirred solution of 4-bromo-2-nitrobenzoic acid (EXAMPLE 5) (3.81 g, 15 mmol) in DMF (30 mL) at 0 C. was added 1,8-diazabicycloundecane (DBU) (10.3 mL, 75 mmol) followed by methyl iodide (4.67 mL, 75 mmol). The reaction mixture was stirred 15 min at 0 C. then allowed to warm to room temperature and stir overnight. The mixture was poured into water and extracted with EtOAc (2*). The combined organic extracts were washed with water (2*), dried (MgSO4), and concentrated in vacuo. The residue was purified by flash chromatography (hexanes/EtOAc) to afford <strong>[158580-57-5]methyl 4-bromo-2-nitrobenzoate</strong> as a pale yellow solid (3.52 g, 90%). |
93% | To a stirred solution of 4-bromo-2-nitrobenzoic acid (3.8 g, 15 mmol) in DMF (30 mL) at 0 C. was added 1,8-diazabicyclo[5.4.0]undec-7-ene (DBU) (10.0 mL, 75.0 mmol) followed by iodomethane (4.7 mL, 75 mmol). The reaction mixture was stirred 15 min at 0 C., then was allowed to warm to room temperature and was stirred overnight. The mixture was poured into H2O and extracted with EtOAc (2×). The combined organic extracts were washed with H2O (2×), dried (MgSO4), and concentrated in vacuo. The residue was purified by flash chromatography (hexanes/EtOAc) to afford <strong>[158580-57-5]methyl 4-bromo-2-nitrobenzoate</strong> as a pale yellow solid (3.52 g, 0.90%). To a solution of the nitrobenzoate (3.52 g, 13.5 mmol) in 1:1 EtOAc/DCM (30 mL) at room temperature was added SnCl2.2H2O (15 g, 67 mmol). The reaction mixture was allowed to stir overnight. The solvents were evaporated in vacuo, and the residue was partitioned between satd. aq. NaHCO3 and DCM. The layers were separated, and the aqueous layer was further extracted with DCM (2×). The combined organic layers were dried (MgSO4) and concentrated in vacuo to provide the pure aminobenzoate as a white solid (2.89 g, 93%). 1H NMR (400 MHz, CDCl3): 7.70 (d, J=8.6 Hz, 1H), 6.84 (d, J=1.9 Hz, 1H), 6.75 (dd, J=8.6, 1.9 Hz, 1H), 5.78 (br s, 2H), 3.86 (s, 3H). | |
93% | With tin(ll) chloride; In dichloromethane; ethyl acetate; at 20℃; for 18h;Product distribution / selectivity; | B. Methyl 2-amino-4-bromobenzoate.; To a stirred solution of 4-bromo-2-nitrobenzoic acid (3.81 g, 15 mmol) in DMF (30 mL) at 0 C. was added 1,8-diazabicycloundecane (DBU; 10.3 mL, 75 mmol) followed by Mel (4.67 mL, 75 mmol). The mixture was stirred for 15 min at 0 C., then was allowed to warm to rt and was stirred overnight. The mixture was poured into water and extracted with EtOAc (2×). The combined organic extracts were washed with water (2×), dried (MgSO4), and concentrated. The residue was purified by flash chromatography (hexanes/EtOAc) to afford <strong>[158580-57-5]methyl 4-bromo-2-nitrobenzoate</strong> as a pale yellow solid (3.52 g, 90%). To a solution of the nitrobenzoate (3.52 g, 13.5 mmol) in 1:1 EtOAc/DCM (30 mL) at rt was added SnCl2.2H2O (15.27 g, 67 mmol). After 18 h, the mixture was concentrated, diluted with satd. aq. NaHCO3, and extracted with DCM (3×). The combined organic layers were dried (MgSO4) and concentrated to provide the desired aminobenzoate as a white solid (2.89 g, 93%). 1H NMR (400 MHz, CDCl3): 7.70(d, J=8.6, 1H), 6.84 (d, J=1.9, 1H), 6.75 (dd, J=8.6, 1.9, 1H), 5.78 (br s, 2H), 3.86 (s, 3H). |
85% | With iron; acetic acid; at 20℃; for 2h; | To a solution of 1A (1.0 g, 3.85 mmol) in Acetic Acid (5 mL) was added iron powder (0.430 g, 7.69 mmol) and allowed to stir for 2 h at room temperature. Then reaction mixture was basified using 10% sodium carbonate (30 mL) and extracted with ethyl acetate (2*200 mL). The combined organic layer was dried over sodium sulfate and concentrated under reduced pressure. The crude sample was purified by flash chromatography (5% Ethyl acetate: Pet ether; 12 g silica gel column) to afford 1B (off white solid 0.75 g, 3.26 mmol, 85% yield). LC-MS Anal. Calc'd for C8H8BrNO2 228.9, found [M+H] 230.3, Tr=0.98 min (Method DM) |
84% | Step 2. Preparation of Methyl 2-amino-4-bromobenzoate Add tin (II) chloride (65.9 g, 292 mmol) to a suspension of methyl 4-bromo-2- nitrobenzoate (15.2 g, 58.4 mmol) in concentrated hydrochloric acid (120 mL) at room temperature and stir for 24 h. Slowly pour the mixture into water (700 mL) and adjust the pH to 9 with solid potassium hydroxide. Filter the white suspension through Celite, then stir the filter cake with ethyl acetate and filter that suspension. Separate the filtrate and extract the aqueous layer with ethyl acetate (200 mL). Combine the organic layers, dry over sodium sulfate, filter and remove the solvent under reduced pressure to afford the title compound as an off-white solid (11.3 g, 84 %) | |
Iron powder 2.6g was added to a mixed solution of methanol 20mL and acetic acid 20mL of <strong>[158580-57-5]methyl 4-bromo-2-nitrobenzoate</strong> 4.0g, it was heated and refluxed for 3 hours. After the reaction mixture was cooled to room temperature, saturated sodium hydrogen carbonate aqueous solution and ethyl acetate were added to it, and insoluble matter was filtrated. The organic layer was separated and collected, dried over anhydrous magnesium sulfate after sequential washing with saturated sodium hydrogen carbonate aqueous solution and saturated sodium chloride aqueous solution, and solvent was removed under reduced pressure. Hexane was added to the obtained residue, solid matter was filtrated to give methyl 2-amino-4-bromobenzoate 2.0g of white solid. 1H-NMR(CDCl3) delta value: 3.89(3H,s),4.20(2H,s),7.26(1H,dd,J=8.3,2.1Hz),7.43(1H,d ,J=2.1Hz),7.47(1H,d,J=8.3Hz). |
Yield | Reaction Conditions | Operation in experiment |
---|---|---|
97% | With caesium carbonate; In N,N-dimethyl-formamide; at 20℃; | Compound 7 A (10.0 g, 40.7 mmol) was dissolved in DMF (100 mL). Cs2CO3 (27.0g, 81.3 mmol) and methyl iodide (7.60 mL, 122.0 mmol) were added. The solution was stirred at room temperature overnight. EtOAc (250 mL) and water (100 mL) were added. The organic phase was separated and washed with water (100 mL) three times and brine (50 mL), then dried over Na2SO4) filtered, and concentrated using a rotary evaporator. The product was dried under vacuum to give compound 7B (10.3 g, 97%). |
94% | With potassium carbonate; In N,N-dimethyl-formamide; at 80℃; for 3h; | Example I-XVIIPreparation of Compound 321General Procedure I-ESTo a mixture of 4-bromo-2-nitrobenzoic acid (10 g, 41 mmol) and K2CO3 (11.3 g, 82 mmol) in 100 mL of DMF was added CH3I (7.1 g, 50 mmol) dropwise and the mixture was stirred at 80 C. for 3 hrs. After cooling to r.t, the mixture was filtered, the filtrated was concentrated under reduced pressure to remove DMF, and the residue was dissolved with EtOAc (50 mL), washed with water (50 mL), brine (50 mL), dried over anhydrous Na2SO4 and concentrated in vacuo. The crude product was purified by column chromatography to give methyl 4-bromo-2-nitrobenzoate (I-XVIIa, 10 g, yield 94%). 1H NMR (400 MHz, CDCl3) delta 8.02 (s, 1H), 7.81 (d, J=8.0 Hz, 1H), 7.66 (d, J=8.0 Hz, 1H), 3.92 (s, 3H). |
94% | With potassium carbonate; In N,N-dimethyl-formamide; at 80℃; for 3h; | To a mixture of 4-bromo-2-nitrobenzoic acid (10 g, 41 mmol, 1 eq) and K2CO3 (11.3 g, 82 mmol, 2 eq) in 100 mL of DMF was added CH3I (7.1 g, 50 mmol, 1.2 eq) dropwise and the mixture was stirred at 80 C for 3 hrs. After cooling to rt, the mixture was filtered, the filtrated was poured into water and extracted with EtOAc (150 mL x 3), washed with water (150 mL x 3) and brine (150 mL x 2), dried over anhydrous Na2SO4 and concentrated in vacuo. The crude product was purified by column chromatography to give methyl 4-bromo-2-nitrobenzoate (10 g, 94%). 1HNMR (300 MHz, DMSO-d6): G 8.34 (s, 1H), 8.08- 8.05 (m, 1 H), 7.85- 7.82 (m, 1 H), 3.85 (s, 3 H). |
94.2% | With caesium carbonate; In N,N-dimethyl-formamide; at 20℃; for 16h; | To a solution of compound 267a (5 g, 4.07 mmol), 4-bromo-2-nitrobenzoic acid in N, N-dimethylformamide (50 mL), cesium carbonate (13.5 g, 40.5 mmol) and methyl iodide (3.8 mL, 61 mmol).The mixture was stirred at room temperature for 16 hours, then the mixture was concentrated under reduced pressure to remove some solvents, water was added to the residue and extracted with ethyl acetate (160 mL × 2), and washed with saturated brine (60 mL × 3),After drying over anhydrous sodium sulfate, the filtrate was concentrated under reduced pressure, and the residue was purified by silica gel chromatography (petroleum ether: ethyl acetate = 91: 9) to obtain a white solid compound 267b, namely 4-bromo-2-nitrobenzene Methyl formate (4.98 g, 94.2% yield. |
90% | With 1,8-diazabicyclo[5.4.0]undec-7-ene; In DMF (N,N-dimethyl-formamide); at 0 - 20℃; | A. Methyl 2-amino-4-bromobenzoate To a stirred solution of 4-bromo-2-nitrobenzoic acid (EXAMPLE 5) (3.81 g, 15 mmol) in DMF (30 mL) at 0 C. was added 1,8-diazabicycloundecane (DBU) (10.3 mL, 75 mmol) followed by methyl iodide (4.67 mL, 75 mmol). The reaction mixture was stirred 15 min at 0 C. then allowed to warm to room temperature and stir overnight. The mixture was poured into water and extracted with EtOAc (2*). The combined organic extracts were washed with water (2*), dried (MgSO4), and concentrated in vacuo. The residue was purified by flash chromatography (hexanes/EtOAc) to afford methyl 4-bromo-2-nitrobenzoate as a pale yellow solid (3.52 g, 90%). |
90% | With 1,8-diazabicyclo[5.4.0]undec-7-ene; In N,N-dimethyl-formamide; at 0 - 20℃; | B. Methyl 2-amino-4-bromobenzoate. ; To a stirred solution of 4-bromo-2-nitrobenzoic acid (3.81 g, 15 mmol) in DMF (30 mL) at 0 C. was added 1,8-diazabicycloundecane (DBU; 10.3 mL, 75 mmol) followed by Mel (4.67 mL, 75 mmol). The mixture was stirred for 15 min at 0 C., then was allowed to warm to rt and was stirred overnight. The mixture was poured into water and extracted with EtOAc (2×). The combined organic extracts were washed with water (2×), dried (MgSO4), and concentrated. The residue was purified by flash chromatography (hexanes/EtOAc) to afford methyl 4-bromo-2-nitrobenzoate as a pale yellow solid (3.52 g, 90%). To a solution of the nitrobenzoate (3.52 g, 13.5 mmol) in 1:1 EtOAc/DCM (30 mL) at rt was added SnCl2.2H2O (15.27 g, 67 mmol). After 18 h, the mixture was concentrated, diluted with satd. aq. NaHCO3, and extracted with DCM (3×). The combined organic layers were dried (MgSO4) and concentrated to provide the desired aminobenzoate as a white solid (2.89 g, 93%). 1H NMR (400 MHz, CDCl3): 7.70(d, J=8.6, 1H), 6.84 (d, J=1.9, 1H), 6.75 (dd, J=8.6, 1.9, 1H), 5.78 (br s, 2H), 3.86 (s, 3H). |
90 - 98% | With 1,8-diazabicyclo[5.4.0]undec-7-ene; In N,N-dimethyl-formamide; at 0 - 20℃; for 48.25 - 72.25h;Product distribution / selectivity; | Example 62:; N-[7-ethyI-6-(l-methyI-lH-pyrazol-4-yl)-2,4-dioxo-l,4-dihydro-2H-quinazoIin-3-yI]- methanesulfonamide; 4-Bromo-2-nitro-benzoic acid methyl ester; To a solution of 4-bromo-2-nitrobenzoic acid (25.3 g, 103 mmol) in DMF (200 mL) at 0 0C were added DBU (79.1 mL, 514.8 mmol) and MeI (32.2 mL, 515 mmol). The reaction mixture was stirred for 15 min at this temperature and for 72 h at r.t. The mixture was poured into water and extracted with EtOAc (2X). The combined organic layers were washed with water (2X), dried (Na2SO4) and the solvent was removed in vacuo. The residue was purified by flash chromatography (silica gel, 7:3 hexanes:EtOAc) to provide the title compound (26.24 g, 98%) as a yellow oil.; Example 71:; N-[7-(l,l-difluoro-ethyl)-6-(2-isopropyl-2H-pyrazol-3-yl)-2,4-dioxo-l,4-dihydro-2H- quinazolin-3-yl]-methanesulfbnamide; 4-Bromo-2-nitro-benzoic acid methyl ester; To solution of 4-bromo-2-nitro-benzoic acid (9 g, 36.58 mmol) in dimethylforrnamide (36 mL) cooled to 0 0C were added l,8-diazabicyclo[5.4.0]und-7-ene (28.09 mL, 182.9 mmol) and MeI (11.4 mL, 182.5 mmol). The reaction mixture was stirred at 0 0C for 15 min and at r.t. for 48 h. The mixture was poured into water and extracted with EtOAc (2X). The combined organic phases were washed with water (2X), dried (Na2SO4) and concentrated to dryness. The crude product was purified by flash chromatography (hexanes to EtOAc / hexanes (4:6)) to give 4-bromo-2-nitro-benzoic acid methyl ester (8.62 g, 33.147 mmol, 90%). 1H-NMR (CDCl3, 400 MHz) 8.02 (s, 1 H), 7.81 (dd, J= 2.3, 10.5Hz IH), 7.66 (d, J= 8.2 Hz, IH), 3.92 (s, 3H). |
78% | With potassium carbonate; In N,N-dimethyl-formamide; at 80℃; for 3h; | To a solution of 4-bromo-2-nitrobenzoic acid (10 g, 40.6 mmol) in DMF (100 mL) was added potassium carbonate (11.24 g, 81 mmol) followed by methyl iodide (3.30 mL, 52.8 mmol) dropwise. The mixture was stirred at 80 C. for 3 h. After cooling to room temperature, the mixture was filtered and residue was dissolved in ethyl acetate (2*200 mL). The organic layer was washed with water (200 mL) followed by brine (100 mL), dried over anhydrous sodium sulfate and concentrated under reduced pressure. The crude sample was purified by flash chromatography (5% Ethyl acetate: Pet ether; 80 g silica gel column) to afford 1A (off white solid, 8.2 g, 31.5 mmol, 78% yield). 1H NMR (400 MHz, DMSO-d6) delta 8.35 (d, J=2.0 Hz, 1H), 8.07 (dd, J=8.0, 1.6 Hz, 1H), 7.84 (d, J=8.0 Hz, 1H), 3.85 (s, 3H). |
0.90% | With 1,8-diazabicyclo[5.4.0]undec-7-ene; In DMF (N,N-dimethyl-formamide); at 0 - 20℃; | To a stirred solution of 4-bromo-2-nitrobenzoic acid (3.8 g, 15 mmol) in DMF (30 mL) at 0 C. was added 1,8-diazabicyclo[5.4.0]undec-7-ene (DBU) (10.0 mL, 75.0 mmol) followed by iodomethane (4.7 mL, 75 mmol). The reaction mixture was stirred 15 min at 0 C., then was allowed to warm to room temperature and was stirred overnight. The mixture was poured into H2O and extracted with EtOAc (2×). The combined organic extracts were washed with H2O (2×), dried (MgSO4), and concentrated in vacuo. The residue was purified by flash chromatography (hexanes/EtOAc) to afford methyl 4-bromo-2-nitrobenzoate as a pale yellow solid (3.52 g, 0.90%). To a solution of the nitrobenzoate (3.52 g, 13.5 mmol) in 1:1 EtOAc/DCM (30 mL) at room temperature was added SnCl2.2H2O (15 g, 67 mmol). The reaction mixture was allowed to stir overnight. The solvents were evaporated in vacuo, and the residue was partitioned between satd. aq. NaHCO3 and DCM. The layers were separated, and the aqueous layer was further extracted with DCM (2×). The combined organic layers were dried (MgSO4) and concentrated in vacuo to provide the pure aminobenzoate as a white solid (2.89 g, 93%). 1H NMR (400 MHz, CDCl3): 7.70 (d, J=8.6 Hz, 1H), 6.84 (d, J=1.9 Hz, 1H), 6.75 (dd, J=8.6, 1.9 Hz, 1H), 5.78 (br s, 2H), 3.86 (s, 3H). |
Yield | Reaction Conditions | Operation in experiment |
---|---|---|
78% | With sulfuric acid; In water; for 16h;Heating / reflux; | Step 1. Preparation of Methyl 4-bromo-2-nitrobenzoate Add concentrated sulfuric acid (7 mL) to a solution of commercially available 4- bromo-2-nitrobenzoic acid (25.0 g, 102 mmol) in methanol (150 mL), and heat at reflux for 16 hours. Cool the reaction to room temperature and pour into water (500 mL) and adjust the pH of the suspension to 9 with solid sodium carbonate. Extract the solution with ethyl acetate (2 x 250 mL), then combine the organic extracts and wash with brine (100 mL), dry over sodium sulfate, filter and remove the solvent under reduced pressure to afford the title compound as a pale amber oil, which crystallizes upon standing (20.5 g, 78%) |
With sulfuric acid; for 4h;Reflux; | (Example 22-1) To a methanol solution (50 ml) of 4-bromo-2-nitrobenzoic acid (2.54 g) was added concentrated sulfuric acid (1.0 ml), followed by heating at reflux for 4 hours. The reaction solution was concentrated under reduced pressure, and water (20 ml) was added to the residue. Under ice cooling, 5 N aqueous sodium hydroxide solution (2.0 ml) and a saturated aqueous sodium hydrogen carbonate solution were added, and extracted with dichloromethane. The organic layer was washed with saturated sodium chloride solution, dried over anhydrous sodium sulfate, and concentrated under reduced pressure. The resulting residue was purified by silica gel column chromatography to afford methyl 4-bromo-2-nitrobenzoate (619 mg). 1H NMR (500 MHz, CDCl3) delta: 3.95 (s, 3H), 7.69 (d, 1H, J = 8.3 Hz), 7.84 (dd, 1H, J = 8.3, 2.0 Hz), 8.05 (d, 1H, J = 2.0 Hz). |
Yield | Reaction Conditions | Operation in experiment |
---|---|---|
75% | With bromine; dibromoisocyanuric acid; In dichloromethane; at 20℃; for 24h;UV-irradiation; | General procedure: EXAMPLE 6 Bromoisocyanurate induced radical bromodecarboxylation of (0335) arenecarboxylic acids bromoisocyanurate (0336) ArCO H ArBr (0337) 2 hv (0338) [00139] A mixture of arenecarboxylic acid ArC02H (1 mmol), bromoisocyanurate, additive and solvent (10 mL) was stirred under fluorescent room light (FL) or warm-white 3 W LED (LL) irradiation (hv). The reaction mixture washed with 1 M aq Na2S03, dried over Na2S04, filtered through short neutral alumina pad and concentrated in vacuo to yield crude bromoarene ArBr. Optionally, the crude bromide was purified by chromatography on silica gel. The results are presented in Table 5. |
methyl 4-bromo-2-nitrobenzoate m.p. 41-43 C.; |
Yield | Reaction Conditions | Operation in experiment |
---|---|---|
With potassium carbonate; In acetone; at 20 - 50℃; for 1h; | To acetone 40mL solution of 4-bromo-2-nitrobenzoic acid 4.0g were added potassium carbonate 3.4g and dimethylsulfate 2.3mL at room temperature, and it was stirred at 50C for 1 hour. After the reaction mixture was cooled to room temperature, the solvent was removed under reduced pressure. Water and ethyl acetate were added to the obtained residue. The organic layer was separated and collected, dried over anhydrous magnesium sulfate after sequential washing with saturated sodium hydrogen carbonate aqueous solution, 1.0mol/L hydrochloric acid and saturated sodium chloride aqueous solution, and the solvent was removed under reduced pressure to give methyl 4-bromo-2-nitrobenzoate 4.1g of white solid. 1H-NMR(CDCl3) delta value: 3.97(3H,s),7.85(1H,d,J=8.3Hz),8.07(1H,dd,J=8.3,2.0Hz),8 .47(1H,d,J=2.0Hz). |
Yield | Reaction Conditions | Operation in experiment |
---|---|---|
47% | With racemic-2-(di-tert-butylphosphino)-1,1?-binaphthyl; caesium carbonate;palladium diacetate; In toluene; at 70℃; for 48h; | Pd(OAc)2 (43 mg, 0.19 mmol), racemic-2-(di-f-butylphosphino)-1,1'-binaphthyl (92 mg, 0.23 mmol), and Cs2CO3 (1.88 g, 5.76 mmol) were placed in a 50 mL flask. The flask was placed under vacuum for 2 minutes and refilled with N2. Compound 7B (1.00 g, 3.84 mmol) and MeOH (0.311 mL, 7.69 mmol) were dissolved in toluene (10 mL). The resulting solution was added to the above flask by pipette. The reaction mixture was stirred at 70 C oil bath for 48 hours. After cooling to room temperature, the solid was filtered and the solvent was removed using a rotary evaporator. The product was isolated by silica gel chromatography (Hexane/EtOAc 20:1 to 10:1) to give compound 7C (380 mg, 47%). |
Yield | Reaction Conditions | Operation in experiment |
---|---|---|
100% | bis-triphenylphosphine-palladium(II) chloride; In 1,4-dioxane; at 80℃; for 18h; | 2-Nitro-4-vinyl-benzoic acid methyl ester; To a solution of <strong>[158580-57-5]4-bromo-2-nitro-benzoic acid methyl ester</strong> (I g, 3.85 mmol) in dioxane (5 mL) were added tributylvmyltin (1.7 mL, 5.76 mmol) and Pd(Ph3P)2Cl2 (275.4 mg, 0.385 mmol). The reaction mixture was stirred at 800C for 18 h, was cooled to r.t. and was diluted with EtOAc. After removal of the precipitate by filtration, the solution was concentrated in vacuo. The residue was purified by flash chromatography (silica gel, hexanes ? 1:1 hexanes:EtOAc) to provide the title compound (820 mg, 100%, 97% purity by HPLC) as a yellow oil. ESI-MS: m/z 208.2 [M+H]+, rt 5.14 min. |
Yield | Reaction Conditions | Operation in experiment |
---|---|---|
With potassium carbonate; dimethyl sulfate; In water; ethyl acetate; acetone; | Referential Example 1 To 40 mL of acetone solution containing 4.0 g of 4-bromo-2-nitrobenzoic acid, 3.4 g of potassium carbonate and 2.3 mL of dimethyl sulfate were added at room temperature and stirred at 50C for 1 hour. After the reaction mixture was cooled to room temperature, the solvent was evaporated under reduced pressure. Water and ethyl acetate were added to the obtained residue. The organic layer was separated and dried over anhydrous magnesium sulfate after washed with a saturated sodium hydrogen carbonate aqueous solution, 1.0 mol/L hydrochloric acid and a saturated sodium chloride aqueous solution sequentially, and the solvent was evaporated under reduced pressure to obtain 4.1 g of methyl 4-bromo-2-nitrobenzoate as white solid. 1H-NMR (CDCl3) delta: 3.97 (3H, s), 7.85 (1H, d, J = 8.3 Hz), 8.07 (1H, dd, J = 8.3, 2.0 Hz), 8.47 (1H, d, J = 2.0 Hz). |
Yield | Reaction Conditions | Operation in experiment |
---|---|---|
With sodium bicarbonate; acetic acid; In methanol; hexane; ethyl acetate; | Referential Example 3 2.6 g of iron powder was added to a mixed solution of 20 mL of methanol and 20 mL of acetic acid containing 4.0 g of <strong>[158580-57-5]methyl 4-bromo-2-nitrobenzoate</strong>, and the resulting mixture was heated to reflux for 3 hours. After the reaction mixture was cooled to room temperature, a saturated sodium hydrogen carbonate aqueous solution and ethyl acetate were added and insoluble were removed by filtration. The organic layer was separated and dried over anhydrous magnesium sulfate after washed with a saturated sodium hydrogen carbonate aqueous solution and a saturated sodium chloride aqueous solution sequentially, and the solvent was evaporated under reduced pressure. Hexane was added to the obtained residue and a solid substance was separated by filtration to obtain 2.0 g of methyl 2-amino-4-bromobenzoate as white solid. 1H-NMR (CDCl3) delta: 3.89 (3H, s), 4.20 (2H, s), 7.26 (1H, dd, J = 8.3, 2.1 Hz), 7.43 (1H, d, J = 2.1 Hz), 7.47 (1H, d, J = 8.3 Hz). |
Yield | Reaction Conditions | Operation in experiment |
---|---|---|
With sodium bicarbonate;tetrakis(triphenylphosphine)palladium (0); In ethanol; water; toluene; | Referential Example 7 To a mixed solution of 42 mL of toluene, 16 mL of ethanol and 7.8 mL of water containing 5.2 g of <strong>[158580-57-5]methyl 4-bromo-2-nitrobenzoate</strong>, 2.9 g of dihydroxyphenyl borane, 4.2 g of sodium hydrogen carbonate and 1.1 g of tetrakis(triphenylphosphine)-palladium (0) were added sequentially and the resulting mixture was heated to reflux under nitrogen atmosphere for 2 hours. After the reaction mixture was cooled to room temperature, 1.1 g of tetrakis(triphenylphosphine)palladium (0) was added to the reaction mixture and the resulting mixture was heated to reflux under nitrogen atmosphere for 2 hours. After the reaction mixture was cooled to room temperature, 1.1 g of tetrakis(triphenylphosphine)palladium (0) was added to the reaction mixture and the resulting mixture was heated to reflux under nitrogen atmosphere for 2 hours. After the reaction mixture was cooled to room temperature, water was added. The organic layer was separated and dried over anhydrous magnesium sulfate after washed with 1.0 mol/L hydrochloric acid and a saturated sodium chloride aqueous solution sequentially, and the solvent was evaporated under reduced pressure. The obtained residue was purified with silica gel column chromatography [eluent; hexane:ethyl acetate = 20:1] to obtain 4.8 g of methyl 2-nitro-4-phenylbenzoate as pale yellow oil. 1H-NMR (CDCl3) delta: 3.94 (3H, s), 7.44-7.53 (3H, m), 7.60-7.63 (2H, m), 7.85-7.86 (2H, m), 8.07 (1H, d, J = 1.4 Hz). |
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