Hughes R K, Doyle W A, Chovnick A, Whittle J R, Burke J F, Bray R C
Biochemistry Laboratory, School of Biological Sciences, University of Sussex, Brighton, U.K.
Biochem J. 1992 Jul 15;285 ( Pt 2)(Pt 2):507-13. doi: 10.1042/bj2850507.
The usefulness in structure/function studies of molybdenum-containing hydroxylases in work with rosy mutant strains of Drosophila melanogaster has been investigated. At least 23 such strains are available, each corresponding to a single known amino acid change in the xanthine dehydrogenase sequence. Sequence comparisons permit identification, with some certainty, of regions associated with the iron-sulphur centres and the pterin molybdenum cofactor of the enzyme. Procedures have been developed and rigorously tested for the assay in gel-filtered extracts of the flies, of different catalytic activities of xanthine dehydrogenase by the use of various oxidizing and reducing substrates. These methods have been applied to 11 different rosy mutant strains that map to different regions of the sequence. All the mutations studied cause characteristic activity changes in the enzyme. In general these are consistent with the accepted assignment of the cofactors to the different domains and with the known reactivities of the molybdenum, flavin and iron-sulphur centres. Most results are interpretable in terms of the mutation affecting electron transfer to or from one redox centre only. The activity data provide evidence that FAD and the NAD+/NADH binding sites are retained in mutants mapping to the flavin domain. Therefore, despite some indications from sequence comparisons, it is concluded that the structure of this domain of xanthine dehydrogenase cannot be directly related to that of other flavoproteins for which structural data are available. The data also indicate that the artificial electron acceptor phenazine methosulphate acts at the iron-sulphur centres and suggest that these centres may not be essential for electron transfer between molybdenum and flavin. The work emphasizes the importance of combined genetic and biochemical study of rosy mutant xanthine dehydrogenase variants in probing the structure and function of enzymes of this class.
研究了含钼羟化酶在果蝇玫瑰色突变株研究中的结构/功能研究的实用性。至少有23种这样的菌株可供使用,每种菌株对应于黄嘌呤脱氢酶序列中一个已知的氨基酸变化。序列比较使得能够较为确定地识别与该酶的铁硫中心和蝶呤钼辅因子相关的区域。已经开发并严格测试了在果蝇凝胶过滤提取物中使用各种氧化和还原底物测定黄嘌呤脱氢酶不同催化活性的方法。这些方法已应用于11种不同的玫瑰色突变株,这些突变株定位于序列的不同区域。所有研究的突变都会导致该酶出现特征性的活性变化。一般来说,这些变化与辅因子在不同结构域的公认分配以及钼、黄素和铁硫中心的已知反应性一致。大多数结果可以解释为突变仅影响向一个氧化还原中心或从一个氧化还原中心的电子转移。活性数据提供了证据,表明黄素腺嘌呤二核苷酸(FAD)和烟酰胺腺嘌呤二核苷酸(NAD +)/烟酰胺腺嘌呤二核苷酸还原酶(NADH)结合位点在定位于黄素结构域的突变体中得以保留。因此,尽管序列比较有一些迹象,但得出的结论是,黄嘌呤脱氢酶该结构域的结构与其他有结构数据的黄素蛋白的结构没有直接关系。数据还表明,人工电子受体硫酸甲酯吩嗪作用于铁硫中心,并表明这些中心可能不是钼和黄素之间电子转移所必需的。这项工作强调了对玫瑰色突变型黄嘌呤脱氢酶变体进行遗传和生化联合研究在探究这类酶的结构和功能方面的重要性。