Carbon monoxide and cyanide as intrinsic ligands to iron in the active site of [NiFe]-hydrogenases -: NiFe(CN)2CO, biology's way to activate H2
Carbon monoxide and cyanide as intrinsic ligands to iron in the active site of [NiFe]-hydrogenases -: NiFe(CN)2CO, biology's way to activate H2
复制标题
DOI：
10.1074/jbc.274.6.3331
复制
发表时间：
1999-02-05
影响因子：
4.8
通讯作者：
Albracht, SPJ
中科院分区：
文献类型：
--
作者：
Pierik, AJ;Roseboom, W;Albracht, SPJ
对富含N-15或C-13的Chromatium vinosum的[NiFe]-氢化酶的光谱研究以及化学分析表明，这种酶含有三个不可交换的、内在的、双原子分子作为活性位点的配体，一个一氧化碳分子和两个氰化物基团。结果形成了对在脱硫弧菌（Desulfovibrio gigas）氢化酶的晶体结构中检测到的铁的三种非蛋白配体的解释（Volbeda，A.，Garcin，E.，皮拉斯，C.，De Lacey，A.一、费尔南德斯，V. M.，Hatchikian，E. C.的方法，Frey，M.，和Fontecilla-Camps，J. C.等人（1996）J. Am.化学分析118，12989-12996）和用穆斯堡尔谱观察到的孤亚铁离子的低自旋特征（Surerus，K. K.，陈美，货车兹万，W.，Rusnak，F. M.，科尔克，M.，Duin，E. C.的方法，阿尔布拉赫特湾P.J.，和Munck，E.（1994）Biochemistry 33，4980-4993）。结果不支持基于普通脱硫弧菌[NiFe]-氢化酶的研究的概念（Higuchi，Y.，Yagi，T.，Noritake，Y.（1997）Structure 5，1671-1680），SO是活性位点的配体。氰化物和一氧化碳作为辅基的内在成分的出现在生物学中是前所未有的。
Infrared-spectroscopic studies on the [NiFe]-hydrogenase of Chromatium vinosum enriched in N-15 Or C-13, as well as chemical analyses, show that this enzyme contains three non-exchangeable, intrinsic, diatomic molecules as ligands to the active site, one carbon monoxide molecule and two cyanide groups. The results form an explanation for the three non-protein ligands to iron detected in the crystal structure of the Desulfovibrio gigas hydrogenase (Volbeda, A., Garcin, E., Piras, C., De Lacey, A. I., Fernandez, V. M., Hatchikian, E. C., Frey, M., and Fontecilla-Camps, J. C. (1996) J. Am. Chem. Sec. 118, 12989-12996) and for the low spin character of the lone ferrous iron ion observed with Mossbauer spectroscopy (Surerus, K. K., Chen, M., Van der Zwaan, W., Rusnak, F. M., Kolk, M., Duin, E. C., Albracht, S. P. J., and Munck, E. (1994) Biochemistry 33, 4980-4993). The results do not support the notion, based upon studies of Desulfovibrio vulgaris [NiFe]-hydrogenase (Higuchi, Y., Yagi, T., and Noritake, Y. (1997) Structure 5, 1671-1680), that SO is a ligand to the active site. The occurrence of both cyanide and carbon monoxide as intrinsic constituents of a prosthetic group is unprecedented in biology.