ON THE STRUCTURE OF THE NICKEL IRON SULFUR CENTER OF THE CARBON-MONOXIDE DEHYDROGENASE FROM RHODOSPIRILLUM-RUBRUM - AN X-RAY ABSORPTION-SPECTROSCOPY STUDY

被引:59
作者
TAN, GO
ENSIGN, SA
CIURLI, S
SCOTT, MJ
HEDMAN, B
HOLM, RH
LUDDEN, PW
KORSUN, ZR
STEPHENS, PJ
HODGSON, KO
机构
[1] STANFORD UNIV,DEPT CHEM,STANFORD,CA 94305
[2] STANFORD UNIV,STANFORD SYNCHROTRON RADIAT LAB,STANFORD,CA 94309
[3] UNIV WISCONSIN PARKSIDE,DEPT CHEM,KENOSHA,WI 53141
[4] UNIV WISCONSIN,DEPT BIOCHEM,MADISON,WI 53706
[5] HARVARD UNIV,DEPT CHEM,CAMBRIDGE,MA 02138
[6] UNIV SO CALIF,DEPT CHEM,LOS ANGELES,CA 90089
关键词
NI CARBON MONOXIDE DEHYDROGENASE; RHODOSPIRILLUM-RUBRUN; EDGE AND EXTENDED X-RAY ABSORPTION FINE STRUCTURE SPECTROSCOPY; NI ACTIVE SITE;
D O I
10.1073/pnas.89.10.4427
中图分类号
O [数理科学和化学]; P [天文学、地球科学]; Q [生物科学]; N [自然科学总论];
学科分类号
07 ; 0710 ; 09 ;
摘要
The nickel/iron/sulfur center of the carbon monoxide dehydrogenase (carbon monoxide:(acceptor)oxidoreductase; EC 1.2.99.2) enzyme from Rhodospirillum rubrum (Rr-CODH) was studied by x-ray absorption spectroscopy at the Ni K edge. Extended x-ray absorption fine structure data show that the first Ni coordination shell consists of 2 S atoms at 2.23 angstrom and 2-3 N/O atoms at 1.87 angstrom. The edge structure indicates a distorted tetrahedral or five-coordinate Ni environment in both oxidized and reduced Rr-CODH. By comparing second-shell extended x-ray absorption fine structure data of Rr-CODH to that of (Et4N)3[NiFe3S4(SEt)4], a cubane-type cluster, it was clearly established that Ni in the Rr-CODH center is not involved in the core of a NiFe3S4 cubane duster. One model consistent with the results is a mononuclear Ni2+ site, bridged by S-Cys or sulfide to one or both of the Fe4S4 clusters of the enzyme, with the remaining coordination sites occupied by additional S-Cys or N/O-liganding amino acid residues.
引用
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页码:4427 / 4431
页数:5
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