Alonso M J, Bermejo F, Reglero A, Fernández-Cañón J M, González de Buitrago G, Luengo J M
Departamento de Bioquímica y Biología Molecular, Universidad de León, España.
J Antibiot (Tokyo). 1988 Aug;41(8):1074-84. doi: 10.7164/antibiotics.41.1074.
Different penicillins (phenylacetyl, 2-hydroxyphenylacetyl, 4-hydroxyphenylacetyl, phenoxyacetyl and 2-thiopheneacetylpenicillin) have been synthesized "in vitro" by direct N-acylation of 6-aminopenicillanic acid (6-APA) with the acyl group of several acyl-CoA derivatives. The enzyme that catalyzes these reactions, acyl-CoA: 6-APA acyltransferase of Penicillium chrysogenum, was purified to homogeneity (374-fold) and its amino acid composition is given. This protein accepts as substrates several aliphatic acids and different aromatic acids with the only requirement that an acetyl-CoA moiety must be present in the substrate molecule. Shortening or lengthening of the acyl moiety prevents the 6-APA-N-acylation reaction. The presence of an amino group in the alpha-position of the acetyl group does not allow this molecule to be used as substrate. However, different substitutions in the phenyl group (hydroxylation of the carbons 2 and 4) or its replacement by another aromatic ring (thiophene) were accepted with varying reactions rates in the acylation reaction when a 176-fold purified acyltransferase was employed. The homogeneity pure enzyme accepts as substrate thiophene acetyl-CoA but it did not 2-hydroxyphenyl and 4-hydroxyphenylacetyl-CoA. The presence of an oxygen atom between the aromatic and the acetyl moieties did not affect the catalysis.
通过用几种酰基辅酶A衍生物的酰基对6-氨基青霉烷酸(6-APA)进行直接N-酰化反应,已在“体外”合成了不同的青霉素(苯乙酰青霉素、2-羟基苯乙酰青霉素、4-羟基苯乙酰青霉素、苯氧乙酰青霉素和2-噻吩乙酰青霉素)。催化这些反应的酶,即产黄青霉的酰基辅酶A:6-APA酰基转移酶,已被纯化至同质(纯化了374倍)并给出了其氨基酸组成。该蛋白质可接受多种脂肪酸和不同的芳香酸作为底物,唯一的要求是底物分子中必须存在乙酰辅酶A部分。缩短或延长酰基部分会阻止6-APA的N-酰化反应。乙酰基α位存在氨基会使该分子不能用作底物。然而,当使用纯化了176倍的酰基转移酶时,苯环上的不同取代(碳2和4的羟基化)或被另一个芳香环(噻吩)取代在酰化反应中具有不同的反应速率。同质纯酶可接受噻吩乙酰辅酶A作为底物,但不能接受2-羟基苯乙酰辅酶A和4-羟基苯乙酰辅酶A。芳香基和乙酰基之间存在氧原子不影响催化作用。