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Lipase-catalyzed regioselective hydrolysis of 3(5)-methylpyrazole-N-carboxylates in water-saturated organic solvents

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    • 바이오플라스틱
      1. 플라스틱
    • 바이오정밀화학
      1. 용매
      2. 화학제품
      3. 연료
      4. 기타
    • 화장품용 기능성소재
      1. 계면활성제⁄증점제
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      1. 식품첨가제
논문

Lipase-catalyzed regioselective hydrolysis of 3(5)-methylpyrazole-N-carboxylates in water-saturated organic solvents

학술지

Journal of molecular catalysis. B, Enzymatic

저자명

Wu, An-Chi; Wang, Pei-Yun; Chen, Kuan-Ju; Tsai, Shau-Wei

초록

<P><B>Graphical abstract</B></P><P><ce:figure id='fig0005'></ce:figure></P><P><B>Highlights</B></P><P>&#x025BA; Novozym 435 lipase can effectively separate 3(5)-methylpyrazole-<I>N</I>-carboxylate mixtures <I>via</I> hydrolysis for preparing pure 5-methylpyrazole-<I>N</I>-carboxylate regioisomers. &#x025BA; A change of solvent hydrophobicity, temperature, or water content in MTBE may enhance the lipase activity and regioselectivity. &#x025BA; An introduction of a 1-methyl side-chain or straight alkyl chain longer than propyl in the <I>N</I>-carboxylate moiety also leads to excellent regioselectivity.</P> <P><B>Abstract</B></P><P>Pure <I>N</I>-substituted-azole regioisomers containing substituents on the <I>C</I>-atom of azole ring may exert different biological activities, just like pure enantiomers do in comparison with their antipodes. It is therefore highly desirable that they can be effectively synthesized from their precursors or separated from regioisomeric mixtures. With lipase-catalyzed hydrolysis of (<I>R</I>)-1-phenylethyl 3(5)-methylpyrazole-<I>N</I>-carboxylate mixture (<B>1a</B> and <B>1b</B>) in water-saturated organic solvents as the model system, excellent regioselectivity (<I>V</I><SUB>1<I>a</I></SUB>/<I>V</I><SUB>1<I>b</I></SUB>>100) for 3-methylpyrazole-<I>N</I>-carboxylate (<B>1a</B>) is obtainable when selecting Novozym 435 from <I>Candida antartica</I> lipase B, but not Lipase MY-30 from <I>Candida rugosa</I> and Lipase PS-D from <I>Pseudomonas cepacia</I>, as the biocatalyst. Increasing of solvent hydrophobicity and temperature, or decreasing of water content, may enhance the enzyme activity but not regioselectivity. A change of the 1-phenylethyl moiety to an isopropyl or straight alkyl chain is longer than propyl for other substrates also results in excellent regioselectivity. The biocatalysis is successfully extended to the hydrolysis of (<I>R</I>)-1-phenylethyl 3(5)-methyl-4-bromopyrazole-<I>N</I>-carboxylate mixture (<B>8a</B> and <B>8b</B>) with <I>V</I><SUB>8<I>a</I></SUB>/<I>V</I><SUB>8<I>b</I></SUB>>100 for preparing pure 5-methyl-4-bromopyrazole-<I>N</I>-carboxylate.</P>

발행연도

2012

ISSN

1381-1177

ISSN

1873-3158

74

1

페이지

pp.41-47

주제어

Lipase; Hydrolysis; Regioselectivity; 3(5)-Methylpyrazole-N-carboxylate regioisomers

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논문; 2012-01-01

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