Burgner J W, Ray W J
Biochemistry. 1984 Jul 31;23(16):3620-6. doi: 10.1021/bi00311a008.
The binary complex of NAD and lactate dehydrogenase reacts reversibly with cyanide to produce a complex (E X NAD-CN) whose noncovalent interactions are similar to those in the E X NADH complex (where E is one-fourth of the tetrameric dehydrogenase). The reaction apparently is a simple bimolecular nucleophilic addition at the 4 position of the bound nicotinamide ring; viz., cyanide does not bind to the enzyme prior to reaction. The value of the dissociation constant for E X NAD-CN is about 1 X 10(-6) M and is independent of pH over the range of 6-8. The equilibrium constant for the reaction of cyanide with E X NAD is about 400-fold larger than that for the nonenzymic process after a statistical correction. This increment in Ke is accounted for by a 220-fold increase in the rate of the forward enzymic reaction (20 M-1 s-1) as compared with an approximately 2-fold decrease for the reverse process (9 X 10(-5) s-1). Thus, the increased value of the rate constant for bond formation in the enzymic reaction is attributed to an equilibrium binding effect that is translated almost entirely into a rate effect on that step (bond formation). Since the nonenzymic reaction is sensitive to solvent composition, this equilibrium binding effect likely is produced by environmental effects at the nicotinamide/dehydronicotinamide part of the coenzyme binding site on the enzyme.
NAD与乳酸脱氢酶的二元复合物可与氰化物发生可逆反应,生成一种复合物(E X NAD-CN),其非共价相互作用与E X NADH复合物(其中E是四聚体脱氢酶的四分之一)中的相互作用相似。该反应显然是在结合的烟酰胺环的4位上进行的简单双分子亲核加成反应;即,氰化物在反应前不与酶结合。E X NAD-CN的解离常数约为1×10⁻⁶ M,在6 - 8的pH范围内与pH无关。经统计校正后,氰化物与E X NAD反应的平衡常数比非酶促反应的平衡常数大约400倍。这种平衡常数(Ke)的增加是由于正向酶促反应速率增加了220倍(20 M⁻¹ s⁻¹),而逆向反应速率则下降了约2倍(9×10⁻⁵ s⁻¹)。因此,酶促反应中键形成速率常数的增加值归因于一种平衡结合效应,这种效应几乎完全转化为对该步骤(键形成)的速率效应。由于非酶促反应对溶剂组成敏感,这种平衡结合效应可能是由酶上辅酶结合位点烟酰胺/脱氢烟酰胺部分的环境效应产生的。