Meyer T, Wielckens K, Thiem J, Hilz H
Eur J Biochem. 1984 May 2;140(3):531-7. doi: 10.1111/j.1432-1033.1984.tb08134.x.
The chemical synthesis of adenosine(5') [alpha-thio]diphospho(5')ribofuranosyl-nicotinamide (NAD[S]) is described. The product occurs as a pair of diastereomers with different configuration at the sulfur-bearing phosphorus atom. The diastereomers were separated by high-performance liquid chromatography and their absolute configuration was determined after chemical degradation to the ADP[alpha S] diastereomers and chromatographic comparison with enzymically synthesized ADP[alpha S] diastereomers of known absolute configuration. Additional support for this assignment is based on different rates in the phosphodiesterase-catalyzed hydrolysis. Furthermore the synthesis of [14C]NAD[S] is described. The coenzyme activity of NAD[S] in the reaction with alcohol dehydrogenase from baker's yeast and lactate dehydrogenase from pig heart is very similar to that of beta-NAD. Also, NAD and NAD[S] serve equally well as substrates for NAD glycohydrolase from calf spleen. In contrast, no reaction was detected with NAD pyrophosphorylase, and hydrolysis of the separated NAD[S] diastereomers with snake venom phosphodiesterase showed a 26-fold and a 33-fold slower reaction rate than that of NAD. Nucleotide pyrophosphatase was less sensitive to the S substitution, hydrolyzing NAD[S] 14-times slower than NAD. Poly(ADP-ribose) polymerase from Ehrlich ascites tumor cell nuclei accepted NAD[S] as a substrate but the reaction was significantly slower and approached saturation at much lower values than with NAD. Alkaline hydrolysis of the products insoluble in trichloroacetic acid yielded AMP[S] as the main derivative. It is concluded that with NAD[S] as a substrate the nuclear acceptors were nearly exclusively mono(ADP-ribosyl) ated .
描述了腺苷(5')[α-硫代]二磷酸(5')核糖呋喃糖基烟酰胺(NAD[S])的化学合成。产物以一对非对映异构体的形式存在,在含硫磷原子处具有不同的构型。通过高效液相色谱法分离非对映异构体,并在化学降解为ADP[αS]非对映异构体并与已知绝对构型的酶促合成的ADP[αS]非对映异构体进行色谱比较后确定其绝对构型。对该归属的额外支持基于磷酸二酯酶催化水解的不同速率。此外,还描述了[14C]NAD[S]的合成。NAD[S]与面包酵母的乙醇脱氢酶和猪心的乳酸脱氢酶反应中的辅酶活性与β-NAD非常相似。此外,NAD和NAD[S]作为小牛脾脏NAD糖水解酶的底物同样良好。相反,未检测到与NAD焦磷酸化酶的反应,并且用蛇毒磷酸二酯酶水解分离的NAD[S]非对映异构体的反应速率比NAD慢26倍和33倍。核苷酸焦磷酸酶对S取代不太敏感,水解NAD[S]的速度比NAD慢14倍。艾氏腹水肿瘤细胞核中的聚(ADP-核糖)聚合酶接受NAD[S]作为底物,但反应明显较慢,并且在比NAD低得多的值时接近饱和。不溶于三氯乙酸的产物的碱性水解产生AMP[S]作为主要衍生物。得出的结论是,以NAD[S]为底物时,核受体几乎完全是单(ADP-核糖基)化的。