Fox B, Walsh C T
J Biol Chem. 1982 Mar 10;257(5):2498-503.
The flavoprotein mercuric reductase catalyzes the two-electron reduction of mercuric ions to elemental mercury using NADPH as an electron donor. It has now been purified from Pseudomonas aeruginosa PAO9501 carrying the plasmid pVS1. In this plasmid system, where the mer operon is on the transposon Tn501, mercuric reductase comprises up to 6% of the soluble cellular protein upon induction with mercurials. The purification is a rapid (two-step), high yield (80%) procedure. Anaerobic titrations of mercuric reductase with dithionite revealed the formation of a charge transfer complex with an absorbance maximum around 540 nm. Striking spectroscopic similarities to lipoamide dehydrogenase and glutathione reductase were observed. These two enzymes, which catalyze the transfer of electrons between pyridine nucleotides and disulfides, are flavoproteins which contain an oxidation-reduction-active cysteine residue at the active site. The expectation that mercuric reductase contains a similar electron acceptor was confirmed when it was shown that mercuric reductase has the capacity to accept four electrons per FAD-containing subunit, and that two thiols become kinetically titrable by 5,5'-dithiobis-(2-nitrobenzoate) upon reduction with NADPH. These are characteristic features of the disulfide reductase class of flavoproteins. Further similarities with at least one of these enzymes, lipoamide dehydrogenase, include the E/EH2 midpoint potential (-269 mV), fluorescence properties, and extinction coefficients of E and EH2. Preliminary observations relevant to an understanding of the mechanism of mercuric reductase are discussed.
黄素蛋白汞还原酶以NADPH作为电子供体,催化汞离子的双电子还原反应,生成元素汞。目前已从携带质粒pVS1的铜绿假单胞菌PAO9501中纯化出该酶。在这个质粒系统中,汞操纵子位于转座子Tn501上,用汞制剂诱导后,汞还原酶占可溶性细胞蛋白的比例高达6%。该纯化方法快速(两步法)、产率高(80%)。用连二亚硫酸盐对汞还原酶进行厌氧滴定,结果显示形成了一种电荷转移复合物,其最大吸光度约为540 nm。观察到它与硫辛酰胺脱氢酶和谷胱甘肽还原酶在光谱上有显著相似之处。这两种酶催化吡啶核苷酸和二硫化物之间的电子转移,它们都是黄素蛋白,在活性位点含有一个氧化还原活性的半胱氨酸残基。当发现汞还原酶每个含FAD的亚基能够接受四个电子,并且在用NADPH还原后,两个巯基可被5,5'-二硫代双(2-硝基苯甲酸)进行动力学滴定,这证实了人们对汞还原酶含有类似电子受体的预期。这些是黄素蛋白二硫化物还原酶类的特征。与这些酶中的至少一种硫辛酰胺脱氢酶的进一步相似之处包括E/EH2中点电位(-269 mV)、荧光特性以及E和EH2的消光系数。文中还讨论了与理解汞还原酶作用机制相关的初步观察结果。