IspG（GcpE）催化反应中间体的 ENDOR 和 HYSCORE 研究。
An ENDOR and HYSCORE investigation of a reaction intermediate in IspG (GcpE) catalysis.
机构信息
Center for Biophysics and Computational Biology, University of Illinois at Urbana-Champaign, 607 South Mathews Avenue, Urbana, Illinois 61801, USA.
出版信息
J Am Chem Soc. 2011 Jun 8;133(22):8400-3. doi: 10.1021/ja200763a. Epub 2011 May 16.
Abstract
IspG is a 4Fe-4S protein that carries out an essential reduction step in isoprenoid biosynthesis. Using electron-nuclear double resonance (ENDOR) and hyperfine sublevel correlation (HYSCORE) spectroscopies on labeled samples, we have specifically assigned the hyperfine interactions in a reaction intermediate. These results help clarify the nature of the reaction intermediate, supporting a direct interaction between the unique fourth Fe in the cluster and C2 and O3 of the ligand.
摘要
IspG 是一种含有 4 个铁原子和 4 个硫原子的蛋白，在异戊烯基生物合成中执行一个重要的还原步骤。通过对标记样品进行电子-核双共振（ENDOR）和超精细亚层相关（HYSCORE）光谱分析，我们专门对反应中间体中的超精细相互作用进行了分配。这些结果有助于阐明反应中间体的性质，支持簇中独特的第四个铁原子与配体的 C2 和 O3 之间的直接相互作用。
相似文献
1
An ENDOR and HYSCORE investigation of a reaction intermediate in IspG (GcpE) catalysis.IspG（GcpE）催化反应中间体的 ENDOR 和 HYSCORE 研究。
J Am Chem Soc. 2011 Jun 8;133(22):8400-3. doi: 10.1021/ja200763a. Epub 2011 May 16.
2
Organometallic mechanism of action and inhibition of the 4Fe-4S isoprenoid biosynthesis protein GcpE (IspG).4Fe-4S 异戊烯基生物合成蛋白 GcpE（IspG）的有机金属作用机制和抑制作用。
Proc Natl Acad Sci U S A. 2010 Jun 22;107(25):11189-93. doi: 10.1073/pnas.1000264107. Epub 2010 Jun 7.
3
Inhibition of the 4Fe-4S Proteins IspG and IspH: an EPR, ENDOR and HYSCORE Investigation.对4Fe-4S蛋白IspG和IspH的抑制作用：一项电子顺磁共振、电子核双共振和高分辨超精细结构谱研究
Chem Sci. 2014 Apr 1;5(4):1642-1649. doi: 10.1039/C3SC53301H.
4
Electron-nuclear double resonance spectroscopic evidence that S-adenosylmethionine binds in contact with the catalytically active [4Fe-4S](+) cluster of pyruvate formate-lyase activating enzyme.电子-核双共振光谱证据表明，S-腺苷甲硫氨酸与丙酮酸甲酸裂解酶激活酶的催化活性[4Fe-4S](+)簇接触结合。
J Am Chem Soc. 2002 Mar 27;124(12):3143-51. doi: 10.1021/ja012034s.
5
The Active-Site [4Fe-4S] Cluster in the Isoprenoid Biosynthesis Enzyme IspH Adopts Unexpected Redox States during Ligand Binding and Catalysis.在类异戊二烯生物合成酶 IspH 中，活性位点 [4Fe-4S] 簇在配体结合和催化过程中呈现出意想不到的氧化还原状态。
J Am Chem Soc. 2024 Feb 14;146(6):3926-3942. doi: 10.1021/jacs.3c11674. Epub 2024 Jan 30.
6
Structure of the GcpE-HMBPP complex from Thermus thermophilius.嗜热栖热菌中GcpE-HMBPP复合物的结构。
Biochem Biophys Res Commun. 2015 Mar 6;458(2):246-50. doi: 10.1016/j.bbrc.2015.01.088. Epub 2015 Feb 7.
7
Paramagnetic intermediates of (E)-4-hydroxy-3-methylbut-2-enyl diphosphate synthase (GcpE/IspG) under steady-state and pre-steady-state conditions.(E)-4-羟基-3-甲基-2-丁烯基二磷酸合酶（GcpE/IspG）在稳态和预稳态条件下的顺磁中间产物。
J Am Chem Soc. 2010 Oct 20;132(41):14509-20. doi: 10.1021/ja101764w.
8
The electronic structure of the H-cluster in the [FeFe]-hydrogenase from Desulfovibrio desulfuricans: a Q-band 57Fe-ENDOR and HYSCORE study.脱硫脱硫弧菌[FeFe]-氢化酶中H簇的电子结构：一项Q波段57Fe-ENDOR和HYSCORE研究
J Am Chem Soc. 2007 Sep 19;129(37):11447-58. doi: 10.1021/ja072592s. Epub 2007 Aug 28.
9
Pyridine inhibitor binding to the 4Fe-4S protein A. aeolicus IspH (LytB): a HYSCORE Investigation.吡啶抑制剂与 4Fe-4S 蛋白 A. aeolicus IspH（LytB）的结合：HYSCORE 研究。
J Am Chem Soc. 2011 May 4;133(17):6525-8. doi: 10.1021/ja2008455. Epub 2011 Apr 12.
10
Isoprenoid biosynthesis in plant chloroplasts via the MEP pathway: direct thylakoid/ferredoxin-dependent photoreduction of GcpE/IspG.通过MEP途径在植物叶绿体中进行类异戊二烯生物合成：GcpE/IspG的直接类囊体/铁氧还蛋白依赖性光还原。
FEBS Lett. 2006 Mar 6;580(6):1547-52. doi: 10.1016/j.febslet.2006.01.082. Epub 2006 Feb 2.
引用本文的文献
1
Iron-Sulfur Cluster Enzymes of the Methylerythritol Phosphate Pathway: IspG and IspH.2-甲基-D-赤藓糖醇-4-磷酸途径的铁硫簇酶：IspG和IspH。
Biochemistry. 2025 Jun 17;64(12):2544-2555. doi: 10.1021/acs.biochem.4c00714. Epub 2025 May 27.
2
Metalloenzymes involved in carotenoid biosynthesis in plants.参与植物类胡萝卜素生物合成的金属酶。
Methods Enzymol. 2022;671:207-222. doi: 10.1016/bs.mie.2022.01.012. Epub 2022 Feb 11.
3
An [FeS]-Alkyl Cluster Stabilized by an Expanded Scorpionate Ligand.一种由扩展型方酸配体稳定的 [FeS]-烷基簇。
J Am Chem Soc. 2020 Aug 19;142(33):14314-14323. doi: 10.1021/jacs.0c06334. Epub 2020 Aug 6.
4
A Synthetic Model of Enzymatic [FeS]-Alkyl Intermediates.一种酶促[FeS]-烷基中间体的合成模型。
J Am Chem Soc. 2019 Aug 28;141(34):13330-13335. doi: 10.1021/jacs.9b06975. Epub 2019 Aug 16.
5
EPR-Derived Structure of a Paramagnetic Intermediate Generated by Biotin Synthase BioB.EPR 谱学揭示生物素合酶 BioB 生成的顺磁中间物的结构
J Am Chem Soc. 2018 Oct 10;140(40):12947-12963. doi: 10.1021/jacs.8b07613. Epub 2018 Sep 28.
6
Advanced paramagnetic resonance spectroscopies of iron-sulfur proteins: Electron nuclear double resonance (ENDOR) and electron spin echo envelope modulation (ESEEM).铁硫蛋白的高级顺磁共振波谱学：电子核双共振（ENDOR）和电子自旋回波包络调制（ESEEM）。
Biochim Biophys Acta. 2015 Jun;1853(6):1370-94. doi: 10.1016/j.bbamcr.2015.01.025. Epub 2015 Feb 14.
7
Inhibition of the 4Fe-4S Proteins IspG and IspH: an EPR, ENDOR and HYSCORE Investigation.对4Fe-4S蛋白IspG和IspH的抑制作用：一项电子顺磁共振、电子核双共振和高分辨超精细结构谱研究
Chem Sci. 2014 Apr 1;5(4):1642-1649. doi: 10.1039/C3SC53301H.
8
Bioorganometallic chemistry with IspG and IspH: structure, function, and inhibition of the [Fe(4)S(4)] proteins involved in isoprenoid biosynthesis.含IspG和IspH的生物有机金属化学：类异戊二烯生物合成中[Fe(4)S(4)]蛋白的结构、功能及抑制作用
Angew Chem Int Ed Engl. 2014 Apr 22;53(17):4294-310. doi: 10.1002/anie.201306712. Epub 2014 Jan 31.
9
Advanced electron paramagnetic resonance on the catalytic iron-sulfur cluster bound to the CCG domain of heterodisulfide reductase and succinate: quinone reductase.结合异二硫键还原酶和琥珀酸：醌还原酶的 CCG 结构域的催化铁硫簇的高级电子顺磁共振
J Biol Inorg Chem. 2013 Dec;18(8):905-15. doi: 10.1007/s00775-013-1037-x. Epub 2013 Sep 14.
10
Methylerythritol phosphate pathway of isoprenoid biosynthesis.异戊烯醇磷酸途径的类异戊二烯生物合成。
Annu Rev Biochem. 2013;82:497-530. doi: 10.1146/annurev-biochem-052010-100934.
本文引用的文献
1
Structure of the E-1-hydroxy-2-methyl-but-2-enyl-4-diphosphate synthase (GcpE) from Thermus thermophilus.嗜热栖热菌的E-1-羟基-2-甲基丁-2-烯基-4-二磷酸合酶（GcpE）的结构
FEBS Lett. 2011 Feb 4;585(3):447-51. doi: 10.1016/j.febslet.2010.12.012. Epub 2010 Dec 15.
2
Biosynthesis of isoprenoids: crystal structure of the [4Fe-4S] cluster protein IspG.异戊烯基化合物的生物合成：[4Fe-4S]簇蛋白 IspG 的晶体结构。
J Mol Biol. 2010 Dec 10;404(4):600-10. doi: 10.1016/j.jmb.2010.09.050. Epub 2010 Oct 7.
3
Paramagnetic intermediates of (E)-4-hydroxy-3-methylbut-2-enyl diphosphate synthase (GcpE/IspG) under steady-state and pre-steady-state conditions.(E)-4-羟基-3-甲基-2-丁烯基二磷酸合酶（GcpE/IspG）在稳态和预稳态条件下的顺磁中间产物。
J Am Chem Soc. 2010 Oct 20;132(41):14509-20. doi: 10.1021/ja101764w.
4
The structure of formaldehyde-inhibited xanthine oxidase determined by 35 GHz 2H ENDOR spectroscopy.通过 35GHz2HENDOR 光谱学确定的甲醛抑制黄嘌呤氧化酶的结构。
J Am Chem Soc. 2010 Oct 13;132(40):14015-7. doi: 10.1021/ja106432h.
5
Methylerythritol cyclodiphosphate (MEcPP) in deoxyxylulose phosphate pathway: synthesis from an epoxide and mechanisms.甲基赤藓醇磷酸（MEcPP）在脱氧木酮糖磷酸途径中的合成：环氧化物的合成及机制。
Chem Commun (Camb). 2010 Oct 14;46(38):7220-2. doi: 10.1039/c0cc02594a. Epub 2010 Sep 1.
6
Organometallic mechanism of action and inhibition of the 4Fe-4S isoprenoid biosynthesis protein GcpE (IspG).4Fe-4S 异戊烯基生物合成蛋白 GcpE（IspG）的有机金属作用机制和抑制作用。
Proc Natl Acad Sci U S A. 2010 Jun 22;107(25):11189-93. doi: 10.1073/pnas.1000264107. Epub 2010 Jun 7.
7
Bioorganometallic mechanism of action, and inhibition, of IspH.IspH 的生物有机金属作用机制及抑制作用。
Proc Natl Acad Sci U S A. 2010 Mar 9;107(10):4522-7. doi: 10.1073/pnas.0911087107. Epub 2010 Feb 19.
8
Probing the reaction mechanism of IspH protein by x-ray structure analysis.通过 X 射线结构分析探究 IspH 蛋白的反应机制。
Proc Natl Acad Sci U S A. 2010 Jan 19;107(3):1077-81. doi: 10.1073/pnas.0913045107. Epub 2009 Dec 28.
9
IspG converts an epoxide substrate analogue to (E)-4-hydroxy-3-methylbut-2-enyl diphosphate: implications for IspG catalysis in isoprenoid biosynthesis.IspG 将环氧化物底物类似物转化为（E）-4-羟基-3-甲基-2-丁烯基二磷酸：对 IspG 在类异戊二烯生物合成中催化作用的影响。
J Am Chem Soc. 2009 Dec 16;131(49):17734-5. doi: 10.1021/ja907470n.
10
Isoprenoid biosynthesis via the MEP pathway: in vivo Mössbauer spectroscopy identifies a [4Fe-4S]2+ center with unusual coordination sphere in the LytB protein.异戊烯基生物合成途径：体内穆斯堡尔谱学鉴定 LytB 蛋白中具有异常配位环境的 [4Fe-4S]2+中心。
J Am Chem Soc. 2009 Sep 23;131(37):13184-5. doi: 10.1021/ja9012408.
Zotero 插件