Insights into the Mechanistic Role of the [Fe4S4] Cubane in the A-Cluster {[Fe4S4]-(SR)-[NipNid]} of Acetyl-Coenzyme A Synthase

被引:7
作者
Liu, Yi [1 ,2 ]
Wang, Feng [3 ]
Li, Pingwei [4 ]
Tan, Xiangshi [1 ,2 ]
机构
[1] Fudan Univ, Dept Chem, Shanghai 200433, Peoples R China
[2] Fudan Univ, Inst Biomed Sci, Shanghai 200433, Peoples R China
[3] Scripps Res Inst, Dept Chem, La Jolla, CA 92037 USA
[4] Texas A&M Univ, Dept Biochem & Biophys, College Stn, TX 77843 USA
基金
中国国家自然科学基金;
关键词
Fe4S4] cubane; NipNid] site; acetyl-coenzyme A synthase; crystal structure; metalloenzymes; CARBON-MONOXIDE DEHYDROGENASE; COA SYNTHASE; ALPHA-SUBUNIT; CLOSTRIDIUM-THERMOACETICUM; ELECTRONIC-PROPERTIES; METHYL TRANSFER; PROTEIN; NICKEL; MODEL; MOSSBAUER;
D O I
10.1002/cbic.201100101
中图分类号
Q5 [生物化学]; Q7 [分子生物学];
学科分类号
071010 ; 081704 ;
摘要
Cubane revolution: We have constructed various mutants to probe the role of [Fe4S4] cubane. The results show that [Fe4S4] cubane, which is bridged to a [NipNid] center via Cys509 cysteinate in the A-cluster of acetyl-coenzyme A synthase (see figure), modulates the redox properties of the catalytic metal Nip and stabilizes the low valence of Nip through the {[Fe4S4]-(SR)-Nip} "conjugation system". © 2011 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.
引用
收藏
页码:1417 / 1421
页数:5
相关论文
共 39 条
[1]   A quantum chemical study of the reaction mechanism of acetyl-coenzyme A synthase [J].
Amara, P ;
Volbeda, A ;
Fontecilla-Camps, JC ;
Field, MJ .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2005, 127 (08) :2776-2784
[2]   Synthetic analogs for evaluating the influence of N-H•••S hydrogen bonds on the formation of thioester in acetyl coenzyme a synthase [J].
Ariyananda, Piyal W. G. ;
Kieber-Emmons, Matthew T. ;
Yap, Glenn P. A. ;
Riordan, Charles G. .
DALTON TRANSACTIONS, 2009, (22) :4359-4369
[3]   THE CCP4 SUITE - PROGRAMS FOR PROTEIN CRYSTALLOGRAPHY [J].
BAILEY, S .
ACTA CRYSTALLOGRAPHICA SECTION D-BIOLOGICAL CRYSTALLOGRAPHY, 1994, 50 :760-763
[4]   Methylation of carbon monoxide dehydrogenase from Clostridium thermoaceticum and mechanism of acetyl coenzyme A synthesis [J].
Barondeau, DP ;
Lindahl, PA .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 1997, 119 (17) :3959-3970
[5]  
BRADFORD MM, 1976, ANAL BIOCHEM, V72, P248, DOI 10.1016/0003-2697(76)90527-3
[6]   Mossbauer and EPR study of recombinant acetyl-CoA synthase from Moorella thermoacetica [J].
Bramlett, Matthew R. ;
Stubna, Audria ;
Tan, Xiangshi ;
Surovtsev, Ivan V. ;
Munck, Eckard ;
Lindahl, Paul A. .
BIOCHEMISTRY, 2006, 45 (28) :8674-8685
[7]   Inactivation of acetyl-CoA synthase/carbon monoxide dehydrogenase by copper [J].
Bramlett, MR ;
Tan, XS ;
Lindahl, PA .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2003, 125 (31) :9316-9317
[8]   Spectroscopic and computational insights into the geometric and electronic properties of the A-cluster of acetyl-coenzyme A synthase [J].
Brunold, TC .
JOURNAL OF BIOLOGICAL INORGANIC CHEMISTRY, 2004, 9 (05) :533-541
[9]   Ni-Zn-[Fe4-S4] and Ni-Ni-[Fe4-S4] clusters in closed and open subunits of acetyl-CoA synthase/carbon monoxide dehydrogenase [J].
Darnault, C ;
Volbeda, A ;
Kim, EJ ;
Legrand, P ;
Vernéde, X ;
Lindahl, PA ;
Fontecilla-Camps, JC .
NATURE STRUCTURAL BIOLOGY, 2003, 10 (04) :271-279
[10]   A Ni-Fe-Cu center in a bifunctional carbon monoxide dehydrogenase/acetyl-CoA synthase [J].
Doukov, TI ;
Iverson, TM ;
Seravalli, J ;
Ragsdale, SW ;
Drennan, CL .
SCIENCE, 2002, 298 (5593) :567-572