Preparation method of N (tau)-methyl-L-histidine derivative and application of derivative in synthesis of anserine
A technology of histidine and derivatives, applied in the field of preparation of N-methyl-L-histidine derivatives, can solve the problems of difficulty in removing protective groups, high price, poor atom economy and the like
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Embodiment 1
[0040] Step a, preparation of tert-butyl (S)-4-(2-((tert-butoxycarbonyl)amino)-3-methoxy-3-oxypropyl)-1H-imidazolyl-1-carbonate
[0041]
[0042] L-Histidine methyl ester dihydrochloride (10g, 41mmol) was dissolved in 100mL of dichloromethane, and sodium bicarbonate (15.5g, 184.5mmol) was added in batches at 20-30°C. After the addition, 20-30 Stir at °C for 1 hour; cool to 0-10 °C, add di-tert-butyl dicarbonate (26.8 g, 123 mmol) in batches, slowly rise to 20-30 °C, stir for 24 hours, TLC detects that the reaction is complete, filter, and wash with water Slurry with methanol, filter and dry to obtain 12.1 g of white solid with a molar yield of 80%.
[0043] Preparation of step b and step c, N(τ)-methyl-L-histidine methyl ester dihydrochloride
[0044]
[0045] tert-butyl (S)-4-(2-((tert-butoxycarbonyl)amino)-3-methoxy-3-oxypropyl)-1H-imidazolyl-1-carbonate (10g, 27mmol) Dissolve in 100mL acetonitrile, add iodomethane (5.75g, 40.5 mmol) at 20-30°C, raise the temperature...
Embodiment 2
[0054] The preparation of step a, compound (III)
[0055]Dissolve L-histidine methyl ester dihydrochloride (41mmol) in 100mL acetonitrile, add potassium carbonate (41mmol) in batches at 20-30°C, after the addition, stir at 70-80°C for 1 hour; cool to 0-10 °C, benzyl chloroformate (73.8 mmol) was added in portions. Slowly rise to 70-80°C, and after stirring for 12 hours, the reaction is complete as detected by TLC. Filter, wash with water and beat with methanol. After filtering and drying, 12.2 g of white solid was obtained, and the molar yield was 80.7%.
[0056] Preparation of step b and step c, compound (I)
[0057] Methyl (S)-4-(2-((ethyloxycarbonyl)amino)-3-methoxy-3-oxypropyl)-1H-imidazolyl-1-carbonate (27mmol) was dissolved in 100mL In tetrahydrofuran, add dimethyl sulfate (27mmol) and sodium bicarbonate (27mmol) at 20-30°C, raise the temperature to 80-90°C and reflux, stir for 12h, TLC shows that the reaction is basically complete, and the crude product obtained aft...
Embodiment 3
[0064] The preparation of step a, compound (III)
[0065] L-Histidine methyl ester dihydrochloride (41mmol) was dissolved in 100mL of isopropyl acetate, and triethylamine (82mmol) was added in batches at 20-30°C, and stirred at 80-90°C for 1 hour after the addition; After cooling to 0-10°C, fluorenylmethyl chloroformate (102.5 mmol) was added in portions. Slowly rise to 80-90°C, and after stirring for 1 hour, the reaction is complete as detected by TLC. Filter, wash with water and beat with methanol. After filtering and drying, 12.3 g of white solid was obtained, and the molar yield was 81%.
[0066] Preparation of step b and step c, compound (I)
[0067] Isopropyl (S)-4-(2-((isopropyloxycarbonyl)amino)-3-methoxy-3-oxypropyl)-1H-imidazolyl-1-carbonate (27mmol) In 100 mL of ethyl acetate, dimethyl carbonate (54 mmol) and potassium carbonate (54 mmol) were added at 20-30 ° C, the temperature was raised to 80-90 ° C, stirred for 1 h, and the reaction was basically complete as...
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