Ohno Hiraku, Takeda Kazuki, Niwa Satomi, Tsujinaka Tomotaka, Hanazono Yuya, Hirano Yu, Miki Kunio
Department of Chemistry, Graduate School of Science, Kyoto University, Sakyo-ku, Kyoto, Japan.
PLoS One. 2017 May 22;12(5):e0178183. doi: 10.1371/journal.pone.0178183. eCollection 2017.
High-potential iron-sulfur protein (HiPIP) is a soluble electron carrier protein of photosynthetic bacteria with an Fe4S4 cluster. Although structural changes accompanying the electron transfer are important for understanding of the functional mechanism, the changes have not been clarified in sufficient detail. We previously reported the high-resolution crystal structures of HiPIP from a thermophilic purple bacterium Thermochromatium tepidum in the reduced state. In order to perform a detailed comparison between the structures in different redox states, the oxidized structure should also be revealed at high resolution. Therefore, in the present study we performed a crystallographic analysis of oxidized HiPIP and a structural comparison with the reduced form at a high resolution of 0.8 Å. The comparison highlighted small but significant contraction in the iron-sulfur cluster. The changes in Fe-S bond lengths were similar to that predicted by theoretical calculation, although some discrepancies were also found. Almost distances between the sulfur atoms of the iron-sulfur cluster and the protein environment are elongated upon the oxidation. Positional changes of hydrogen atoms in the protein environment, such as on the amide-hydrogen of Cys75 in the proximity of the iron-sulfur cluster, were also observed in the accurate analyses. None of the water molecules exhibited significant changes in position or anisotropy of atomic displacement parameter between the two states, while the orientations of some water molecules were different.
高电位铁硫蛋白(HiPIP)是一种存在于光合细菌中的可溶性电子载体蛋白,含有一个Fe4S4簇。尽管伴随电子转移的结构变化对于理解其功能机制很重要,但这些变化尚未得到足够详细的阐明。我们之前报道过热嗜温紫色细菌嗜热栖热菌中还原态HiPIP的高分辨率晶体结构。为了对不同氧化还原状态下的结构进行详细比较,还需要高分辨率揭示氧化态结构。因此,在本研究中,我们对氧化态HiPIP进行了晶体学分析,并与还原态在0.8埃的高分辨率下进行了结构比较。比较结果突出显示了铁硫簇中虽小但显著的收缩。Fe-S键长的变化与理论计算预测的相似,不过也发现了一些差异。铁硫簇中硫原子与蛋白质环境之间的几乎所有距离在氧化时都会延长。在精确分析中还观察到蛋白质环境中氢原子的位置变化,例如在铁硫簇附近的Cys75酰胺氢上。两种状态之间,没有水分子在位置或原子位移参数的各向异性上表现出显著变化,不过一些水分子的取向有所不同。