A Consensus Mechanism for Radical SAM-Dependent Dehydrogenation? BtrN Contains Two [4Fe-4S] Clusters

被引：65

作者：

Grove, Tyler L. ^{[1
]}

Ahlum, Jessica H. ^{[1
]}

Sharma, Priya ^{[1
]}

Krebs, Carsten ^{[1
,2
]}

Booker, Squire J. ^{[1
,2
]}

机构：

[1] Penn State Univ, Dept Chem, University Pk, PA 16802 USA

[2] Penn State Univ, Dept Biochem & Mol Biol, University Pk, PA 16802 USA

来源：

BIOCHEMISTRY | 2010年 / 49卷 / 18期

基金：

美国国家卫生研究院;

关键词：

S-ADENOSYLMETHIONINE; PROTEIN SUPERFAMILY; FORMYLGLYCINE; SULFATASE; ATSB;

D O I：

10.1021/bi9022126

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：

BtrN catalyzes the two-electron oxidation of the C3 secondary alcohol of 2-deoxy-scyllo-inosamine to the corresponding ketone and is a member of a subclass of radical S-adenosylmethionine (SAM) enzymes called radical SAM (RS) dehydrogenases. Like all RS enzymes, BtrN contains a [4Fe-4S] cluster that delivers an electron to SAM, inducing its cleavage to the common intermediate in RS reactions, the 5'-deoxyadenosyl 5'-radical. In this work, we show that BtrN contains an additional [4Fe-4S] cluster, thought to bind in contact with the substrate to facilitate loss of the second electron in the two-electron oxidation.

引用

页码：3783 / 3785

页数：3

共 13 条

[1] Anaerobic sulfatase-maturating enzymes: Radical SAM enzymes able to catalyze in vitro sulfatase post-translational modification
Benjdia, Alhosna
Leprince, Jerome
Guillot, Alain
Vaudry, Hubert
Rabot, Sylvie
Berteau, Olivier
[J]. JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2007, 129 (12) : 3462 - +
[2] Anaerobic functionalization of unactivated C-H bonds
Booker, Squire J.
[J]. CURRENT OPINION IN CHEMICAL BIOLOGY, 2009, 13 (01) : 58 - 73
[3] Coordination and mechanism of reversible cleavage of S-adenosylmethionine by the [4Fe-4S] center in lysine 2,3-aminomutase
Chen, DW
Walsby, C
Hoffman, BM
Frey, PA
[J]. JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2003, 125 (39) : 11788 - 11789
[4] Post-translational formylglycine modification of bacterial sulfatases by the radical S-adenosylmethionine protein AtsB
Fang, QH
Peng, JH
Dierks, T
[J]. JOURNAL OF BIOLOGICAL CHEMISTRY, 2004, 279 (15) : 14570 - 14578
[5] Frey PA, 2001, ADV PROTEIN CHEM, V58, P1
[6] In vitro characterization of AtsB, a radical SAM formylglycine-generating enzyme that contains three [4Fe-4S] clusters
Grove, Tyler L.
Lee, Kyung-Hoon
St. Clair, Jennifer
Krebs, Carsten
Booker, Squire J.
[J]. BIOCHEMISTRY, 2008, 47 (28) : 7523 - 7538
[7] CORRELATION BETWEEN IONIZATION-CONSTANTS OF ORGANIC FREE-RADICALS AND ELECTROCHEMICAL PROPERTIES OF PARENT COMPOUNDS
RAO, PS
HAYON, E
[J]. ANALYTICAL CHEMISTRY, 1976, 48 (03) : 564 - 568
[8] A NOVEL AMINO-ACID MODIFICATION IN SULFATASES THAT IS DEFECTIVE IN MULTIPLE SULFATASE DEFICIENCY
SCHMIDT, B
SELMER, T
INGENDOH, A
VONFIGURA, K
[J]. CELL, 1995, 82 (02) : 271 - 278
[9] Radical SAM, a novel protein superfamily linking unresolved steps in familiar biosynthetic pathways with radical mechanisms: functional characterization using new analysis and information visualization methods
Sofia, HJ
Chen, G
Hetzler, BG
Reyes-Spindola, JF
Miller, NE
[J]. NUCLEIC ACIDS RESEARCH, 2001, 29 (05) : 1097 - 1106
[10] The iron sulfur protein AtsB is required for posttranslational formation of formylglycine in the Klebsiella sulfatase
Szameit, C
Miech, C
Balleininger, M
Schmidt, B
von Figura, K
Dierks, T
[J]. JOURNAL OF BIOLOGICAL CHEMISTRY, 1999, 274 (22) : 15375 - 15381

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