New compound 1-(diphenyl methylene) amino-2-amino-2-methylmethane, preparation method and application thereof in Anagliptin synthesis
A technology of diphenylmethyleneaminoacetonitrile and diphenylmethylene, which is applied in the application field of the synthesis of new compounds 1-amino-2-amino-2-methylpropane and anagliptin
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Embodiment 1
[0061] Example 1: Compound of formula (II): 2-(diphenylmethylene)amino-2-methylpropionitrile Preparation method 1
[0062]
[0063] At room temperature, dissolve 200 g (907.9 mmol) of dibenzylidene aminoacetonitrile (ie, the compound of formula (Ⅲ)) in 4 L of N,N-dimethylformamide (DMF), cool down to 0°C, and add 109 g (2.724 mol) NaOH, add 387g (2.724mol) methyl iodide liquid dropwise at 0°C for 1 hour, after the dropwise addition, keep the reaction at 0°C for 24 hours, TLC monitors until the compound of formula (Ⅲ) completely disappears; Drop it down to 10°C, and add 4L of water dropwise at this temperature. After the dropwise addition, keep stirring for 0.5h, then filter, wash the filter cake with 200mL of water, and dry at 50°C to obtain a light yellow crystalline solid, which is the formula ( Ⅱ) Compound 176.6g, yield 78%.
[0064] MS: 249 [M+H]
[0065] 1 H NMR (400MHz, DMSO-d 6 ), ppm: 7.37-7.29(m, 6H), 7.25-7.22(m, 2H), 7.16-7.14(dd, J=1.6, J=2.4, 2H), 1.51(s, ...
Embodiment 2
[0066] Example 2: Compound of formula (II): 2-(diphenylmethylene)amino-2-methylpropionitrile Preparation method 2
[0067]
[0068] At room temperature, dissolve 200 g (907.9 mmol) of dibenzylidene aminoacetonitrile (ie, the compound of formula (Ⅲ)) in 4 L of N,N-dimethylformamide (DMF), cool down to 0°C, and add 109 g (2.724 mol) NaOH, add 387g (2.724mol) iodomethane liquid dropwise at 0°C, add dropwise for 1h, after the dropwise addition, keep it warm at 0°C for 0.5h, then rise to 50°C for 6h, TLC monitoring to the raw material formula (Ⅲ) The compound disappears completely; lower the system to 10°C, and add 4L of water dropwise at this temperature. After the dropwise addition, keep stirring for 0.5h, then filter, wash the filter cake with 200mL of water, and dry it at 50°C. A light yellow crystalline solid was obtained, namely 181 g of the compound of formula (II), with a yield of 80%.
Embodiment 3
[0069] Example 3: Compound of formula (II): 2-(diphenylmethylene)amino-2-methylpropionitrile Preparation method 3
[0070]
[0071] At room temperature, dissolve 200 g (907.9 mmol) of dibenzylidene aminoacetonitrile (ie, the compound of formula (Ⅲ)) in 4 L of N,N-dimethylformamide (DMF), cool down to 0°C, and add 109 g (2.724 mol) NaOH, add 387g (2.724mol) methyl iodide liquid dropwise at 0°C, add dropwise for 1h, after the dropwise addition, keep it warm at 0°C for 0.5h, then rise to room temperature for 15h, TLC monitors to the raw material formula ( Ⅲ) The compound disappeared completely; the system was lowered to 10°C, and 4L of water was added dropwise at this temperature. After the dropwise addition, it was kept and stirred for 0.5h, then filtered, and the filter cake was washed with 200mL of water and dried at 50°C to obtain Light yellow crystalline solid, that is, compound of formula (II) 185.7g, yield 82%.
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