Department of Chemistry, University of Massachusetts, Amherst, MA 01003, USA.
Biochemistry. 2013 Jan 8;52(1):84-97. doi: 10.1021/bi300886q. Epub 2012 Dec 24.
The RcnR metalloregulator represses the transcription of the Co(II) and Ni(II) exporter, RcnAB. Previous studies have shown that Co(II) and Ni(II) bind to RcnR in six-coordinate sites, resulting in derepression. Here, the roles of His60, His64, and His67 in specific metal recognition are examined. His60 and His64 correspond to ligands that are important for Cu(I) binding in the homologous Cu(I)-responsive metalloregulator, CsoR. These residues are known to be functionally important in RcnR transcriptional regulation. X-ray absorption spectroscopy (XAS) was used to examine the structure of bound cognate and noncognate metal ions, and lacZ reporter assays were used to assess the transcription of rcnA in response to metal binding in the three His → Cys mutations, H60C, H64C, and H67C. These studies confirm that both Ni(II) and Co(II) use His64 as a ligand. H64C-RcnR is also the only known mutant that retains a Co(II) response while eliminating the response to Ni(II) binding. XAS data indicate that His60 and His67 are potential Co(II) ligands. The effects of the mutations of His60, His64, and His67 on the structures of the noncognate metal ions [Zn(II) and Cu(I)] reveal that these residues have distinctive roles in binding noncognate metals. None of the His → Cys mutants in RcnR confer any response to Cu(I) binding, including H64C-RcnR, where the ligands involved in Cu(I) binding in CsoR are present. These data indicate that while the secondary, tertiary, and quaternary structures of CsoR and RcnR are quite similar, small changes in primary sequence reveal that the specific mechanisms involved in metal recognition are quite different.
RcnR 金属调控蛋白抑制 Co(II)和 Ni(II)外排蛋白 RcnAB 的转录。先前的研究表明,Co(II)和 Ni(II)以六配位方式与 RcnR 结合,导致去阻遏。本研究检验了 His60、His64 和 His67 在特定金属识别中的作用。His60 和 His64 对应于在同源铜(I)响应金属调控蛋白 CsoR 中对 Cu(I)结合很重要的配体。这些残基在 RcnR 转录调控中被认为具有功能重要性。使用 X 射线吸收光谱(XAS)研究了结合的同源和非同源金属离子的结构,并使用 lacZ 报告基因测定评估了三个 His → Cys 突变体(H60C、H64C 和 H67C)中金属结合对 rcnA 转录的影响。这些研究证实 Ni(II)和 Co(II)均使用 His64 作为配体。H64C-RcnR 也是唯一已知的突变体,它保留了对 Co(II)的响应,同时消除了对 Ni(II)结合的响应。XAS 数据表明 His60 和 His67 可能是 Co(II)的配体。His60、His64 和 His67 的突变对非同源金属离子[Zn(II)和 Cu(I)]的结构的影响表明,这些残基在结合非同源金属方面具有独特的作用。RcnR 中的 His → Cys 突变体均未赋予任何对 Cu(I)结合的响应,包括 H64C-RcnR,其中涉及 CsoR 中 Cu(I)结合的配体存在。这些数据表明,虽然 CsoR 和 RcnR 的二级、三级和四级结构非常相似,但一级序列的微小变化表明,涉及金属识别的特定机制有很大的不同。