A Radical Intermediate in Bacillus subtilis QueE during Turnover with the Substrate Analogue 6-Carboxypterin.
A Radical Intermediate in Bacillus subtilis QueE during Turnover with the Substrate Analogue 6-Carboxypterin.
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DOI：
10.1021/jacs.7b10860
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发表时间：
2018-02-07
影响因子：
15
通讯作者：
Britt RD
中科院分区：
文献类型：
--
作者：
Wilcoxen J;Bruender NA;Bandarian V;Britt RD
7-Carboxy-7-deazaguanine (CDG) synthase (QueE), a member of the radical S-deoxyadenosyl-L-methionine (SAM) superfamily of enzymes, catalyzes a radical-mediated ring rearrangement required to convert 6-carboxy-5,6,7,8-tetrahydropterin (CPH4) into CDG, forming the 7-dezapurine precursor to all pyrrolopyrimidine metabolites. Members of the radical SAM superfamily bind SAM to a [4Fe-4S] cluster, leveraging the reductive cleavage of SAM by the cluster to produce a highly reactive 5′-deoxyadenosyl radical which initiates chemistry by H-atom abstraction from the substrate. QueE has recently been shown to use 6-carboxypterin (6-CP) as an alternative substrate, forming 6-deoxyadenosylpterin as the product. This reaction has been proposed to occur by radical addition between 5′-dAdo• and 6-CP, which upon oxidative decarboxylation yields the modified pterin. Here, we present spectroscopic evidence for a kinetically competent 6-CP-dAdo radical. The structure of this intermediate is determined by characterizing its electronic structure by continuous wave and pulse electron paramagnetic resonance spectroscopy.
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影响因子：
14.8
作者：
Dowling, Daniel P.;Bruender, Nathan A.;Young, Anthony P.;McCarty, Reid M.;Bandarian, Vahe;Drennan, Catherine L.
通讯作者：
Drennan, Catherine L.
影响因子：
15
作者：
Mahanta N;Fedoseyenko D;Dairi T;Begley TP
通讯作者：
Begley TP
自由基 SAM 酶进行甲基转移的结构基础。
DOI：
10.1126/science.1205358
发表时间：
2011-05-27
期刊：
Science (New York, N.Y.)
影响因子：
--
作者：
Boal AK;Grove TL;McLaughlin MI;Yennawar NH;Booker SJ;Rosenzweig AC
通讯作者：
Rosenzweig AC
影响因子：
15
作者：
Bruender NA;Grell TA;Dowling DP;McCarty RM;Drennan CL;Bandarian V
通讯作者：
Bandarian V
影响因子：
3.7
作者：
Kulik, Leonid;Lubitz, Wolfgang
通讯作者：
Lubitz, Wolfgang