Beta-aryl thioether substituted alpha, beta-cycloenone derivative as well as preparation method and application thereof
A technology of aryl sulfides and derivatives, which is applied in the synthesis of cycloenone NF-κB inhibitors, α, β-cycloenone derivatives substituted by β-aryl sulfides and their preparation fields, capable of Solve the problems of high toxicity and easy drug resistance
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Embodiment 1
[0099] Synthesis of compound 1,5,5-dimethyl-3-((1-phenyl-1H-tetrazol-5-yl)thio)cyclohex-2-enone, starting from aniline and reacting with carbon disulfide Generate phenyl isothiocyanate, and then condense with sodium azide to obtain the intermediate 1-phenyl-5-mercaptotetrazolium. 5,5-Dimethyl-1,3-cyclohexanedione was chlorinated to obtain 3-chloro-5,5-dimethylcyclohex-2-enone. Compound 1 was obtained after alkylation of 1-phenyl-5-mercaptotetrazolium and 3-chloro-5,5-dimethylcyclohex-2-enone under basic conditions.
[0100] Step 1: Preparation of phenylisothiocyanate
[0101] Dissolve 5 milliliters of aniline and 42 milliliters of triethylamine in 60 milliliters of tetrahydrofuran, and add 4.1 milliliters of carbon disulfide dropwise under the protection of a nitrogen atmosphere. The temperature of the reaction solution is kept at 0-5 degrees during the addition process, and the temperature of the reaction solution rises naturally after the addition. to room temperature and ...
Embodiment 2
[0112] Synthesis of compound 2, 3-((1-phenyl-1H-tetrazol-5-yl)thio)cyclohex-2-enone, 1,3-cyclohexanedione was chlorinated to obtain 3-chloro Cyclohex-2-enone. Compound 2 was obtained after alkylation of 1-phenyl-5-mercaptotetrazole and 3-chlorocyclohex-2-enone under basic conditions.
[0113] Step 1: Preparation of 3-chlorocyclohex-2-enone
[0114] Dissolve 15 grams of 1,3-cyclohexanedione in 40 milliliters of chloroform, carefully add 28.7 milliliters of oxalyl chloride dropwise at room temperature within 30 minutes, reflux for 20 minutes after the addition, cool to room temperature, evaporate the solvent, and the residue 13.7 g of a colorless transparent liquid (20 mmHg, 110°C) was obtained by vacuum distillation with a yield of 79%.
[0115] 1 H NMR (400MHz, CDCl 3 ppm: 6.22 (s, 1H), 2.68 (t, J = 6.1 Hz, 2H), 2.40 (t, J = 6.8 Hz, 2H), 2.14-2.04 (m, 2H).
[0116] Step 2: Preparation of 3-((1-phenyl-1H-tetrazol-5-yl)thio)cyclohex-2-enone
[0117] 1-phenyl-5-mercapto-...
Embodiment 3
[0120] Synthetic compound 3,3-((1-(2-methyl)phenyl-1H-tetrazol-5-yl) thio)cyclohex-2-enone, with 2-methylaniline as raw material, and Carbon disulfide reacts to generate 2-methylphenylisothiocyanate, and then condenses with sodium azide to obtain the intermediate 1-(2-methyl)phenyl-5-mercaptotetrazolium. Compound 3 was obtained after alkylation of 1-(2-methyl)phenyl-5-mercaptotetrazolium and 3-chlorocyclohex-2-enone under basic conditions.
[0121] With reference to the method of Example 1, prepare 1-(2-methyl)phenyl-5-mercaptotetrazolium, then react with 3-chlorocyclohex-2-enone,
[0122] The synthesis process is the same as 1. Yield 65%.
[0123] 1 H NMR (CDCl 3 ) ppm: 7.53(m,1H),7.42(m,2H),7.22(d,1H,J=7.6Hz),6.17(s,1H),2.56(m,2H),2.40(t,2H,J =6.4Hz), 2.08(m,5H). 13 C-NMR (CDCl 3 ) ppm: 195.7, 145.9, 149.5, 135.0, 131.9, 131.8, 131.6, 128.1, 127.3, 126.7, 36.8, 30.4, 22.5, 17.4. HRMS (MALDI): C 14 h 15 N 4 OS, calculated: 287.0961, found: 287.0968.
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