Biran Shai, Gat Yair, Fass Deborah
Department of Structural Biology, Weizmann Institute of Science, Rehovot, Israel.
PLoS One. 2014 Dec 1;9(12):e113431. doi: 10.1371/journal.pone.0113431. eCollection 2014.
The widespread thioredoxin superfamily enzymes typically share the following features: a characteristic α-β fold, the presence of a Cys-X-X-Cys (or Cys-X-X-Ser) redox-active motif, and a proline in the cis configuration abutting the redox-active site in the tertiary structure. The Cys-X-X-Cys motif is at the solvent-exposed amino terminus of an α-helix, allowing the first cysteine to engage in nucleophilic attack on substrates, or substrates to attack the Cys-X-X-Cys disulfide, depending on whether the enzyme functions to reduce, isomerize, or oxidize its targets. We report here the X-ray crystal structure of an enzyme that breaks many of our assumptions regarding the sequence-structure relationship of thioredoxin superfamily proteins. The yeast Protein Disulfide Isomerase family member Eps1p has Cys-X-X-Cys motifs and proline residues at the appropriate primary structural positions in its first two predicted thioredoxin-fold domains. However, crystal structures show that the Cys-X-X-Cys of the second domain is buried and that the adjacent proline is in the trans, rather than the cis isomer. In these configurations, neither the "active-site" disulfide nor the backbone carbonyl preceding the proline is available to interact with substrate. The Eps1p structures thus expand the documented diversity of the PDI oxidoreductase family and demonstrate that conserved sequence motifs in common folds do not guarantee structural or functional conservation.
典型的α-β折叠、存在Cys-X-X-Cys(或Cys-X-X-Ser)氧化还原活性基序,以及在三级结构中与氧化还原活性位点邻接的顺式构型脯氨酸。Cys-X-X-Cys基序位于α-螺旋溶剂暴露的氨基末端,这使得第一个半胱氨酸能够对底物进行亲核攻击,或者底物攻击Cys-X-X-Cys二硫键,具体取决于该酶是发挥还原、异构化还是氧化其靶标的功能。我们在此报告一种酶的X射线晶体结构,该结构打破了我们许多关于硫氧还蛋白超家族蛋白序列-结构关系的假设。酵母蛋白二硫键异构酶家族成员Eps1p在其前两个预测的硫氧还蛋白折叠结构域的适当一级结构位置具有Cys-X-X-Cys基序和脯氨酸残基。然而,晶体结构表明第二个结构域的Cys-X-X-Cys被掩埋,且相邻的脯氨酸处于反式而非顺式异构体。在这些构型中,“活性位点”二硫键和脯氨酸之前的主链羰基均无法与底物相互作用。因此,Eps1p的结构扩展了已记录的PDI氧化还原酶家族的多样性,并表明常见折叠中的保守序列基序并不能保证结构或功能的保守性。