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题名: Higher-Order Human Telomeric G-Quadruplex DNA Metalloenzymes Enhance Enantioselectivity in the Diels-Alder Reaction
作者: Li, Yinghao1, 2;  Jia, Guoqing1;  Wang, Changhao1, 2;  Cheng, Mingpan1, 2;  Li, Can1
关键词: Diels-Alder reaction ;  DNA ;  enantioselective catalysis ;  G-quadruplexes ;  human telomeric DNA ;  metalloenzyme
刊名: CHEMBIOCHEM
发表日期: 2015-03-02
DOI: 10.1002/cbic.201402692
卷: 16, 期:4, 页:618-624
收录类别: SCI ;  IC
文章类型: Article
WOS标题词: Science & Technology ;  Life Sciences & Biomedicine
类目[WOS]: Biochemistry & Molecular Biology ;  Chemistry, Medicinal
研究领域[WOS]: Biochemistry & Molecular Biology ;  Pharmacology & Pharmacy
英文摘要: Short human telomeric (HT) DNA sequences form single G-quadruplex (G(4)) units and exhibit structure-based stereocontrol for a series of reactions. However, for more biologically relevant higher-order HT G(4)-DNAs (beyond a single G(4) unit), the catalytic performances are unknown. Here, we found that higher-order HT G(4)-DNA copper metalloenzymes (two or three G(4) units) afford remarkably higher enantioselectivity (>90% ee) and a five- to sixfold rate increase, compared to a single G(4) unit, for the Diels-Alder reaction. Electron paramagnetic resonance (EPR) and enzymatic kinetic studies revealed that the distinct catalytic function between single and higher-order G(4)-DNA copper metalloenzymes can be attributed to different Cu-II coordination environments and substrate specificity. Our finding suggests that, like protein enzymes and ribozymes, higher-order structural organization is crucial for G(4)-DNA-based catalysis.
关键词[WOS]: ASYMMETRIC CATALYSIS ;  K+ SOLUTION ;  CIRCULAR-DICHROISM ;  BINDING-SITE ;  CD SPECTRA ;  RIBOZYME ;  WATER ;  POLYMORPHISM ;  STABILITY ;  MULTIMERS
语种: 英语
WOS记录号: WOS:000350138700012
Citation statistics: 
内容类型: 期刊论文
URI标识: http://cas-ir.dicp.ac.cn/handle/321008/145978
Appears in Collections:中国科学院大连化学物理研究所_期刊论文

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作者单位: 1.Chinese Acad Sci, Dalian Inst Chem Phys, State Key Lab Catalysis, Dalian 116023, Peoples R China
2.Univ Chinese Acad Sci, Beijing 100049, Peoples R China

Recommended Citation:
Li, Yinghao,Jia, Guoqing,Wang, Changhao,et al. Higher-Order Human Telomeric G-Quadruplex DNA Metalloenzymes Enhance Enantioselectivity in the Diels-Alder Reaction[J]. CHEMBIOCHEM,2015,16(4):618-624.
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