Journal
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
Volume 139, Issue 23, Pages 7768-7779Publisher
AMER CHEMICAL SOC
DOI: 10.1021/jacs.7b00648
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Funding
- National Natural Science Foundation of China [21503229, 11334004]
- Fundamental Research Funds for the Central Universities [020514380070]
- National Basic Research Program of China (973 Program) [2013CB834100]
- State Key Laboratory of Analytical Chemistry for Life Science, Nanjing University
- MEXT
- Hirao Taro Foundation of KONAN GAKUEN for Academic Research, Japan
- Inserm (ATIP-Avenir Grant) [R12086GS]
- Conseil Regional d'Aquitaine [20121304005]
- EU [FP7-PEOPLE-2012-CIG-333611]
- Conseil Regional d'Aquitaine
- Agence Nationale de la Recherche [ANR-12-IS07-0001, ANR-12-BSV8-0008-01, ANR-10-NANO-04-03]
- SYMBIT project - ERDF [CZ.02.1.01/0.0/0.0/15_003/0000477]
- Grants-in-Aid for Scientific Research [15H03840, 17K05941, 16H02283, 16K14042] Funding Source: KAKEN
- Agence Nationale de la Recherche (ANR) [ANR-12-IS07-0001] Funding Source: Agence Nationale de la Recherche (ANR)
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To understand the role of ribose G-quartets and how they affect the properties of G-quadruplex, structures, we studied three systems in which one, two, three, or four deoxyribose G-quartets were substituted-with ribose G-quartets. These systems were a parallel DNA intramolecular G-quadruplex, d(TTGGG-TGGGTTGGGTGGGTT), and two tetramolecular G-quadruplexes, d(TGGGT) and cl(TQGGGT). Thermal denaturation experiments revealed that ribose G-quartets have position dependent and cumulative effects on G-quadruplex stability. An unexpected destabilization was observed when rG quartets were presented at the 5'-end of the G stack. This observation challenges the general belief that RNA residues, stabilize G-quadruplexes. Furthermore, in contrast to past proposals, hydration is not the main factor determining the stability of our RNA/DNA chimeric G-quadruplexes. Interestingly, the presence of rG residues in a central G-quartet facilitated the formation of additional tetramolecular G-quadruplex topologies showing positive circular dichroism signals at 295 nm. 2D NMR analysis of the tetramolecular TGgGGT (lowercase letter indicates ribose) indicates that Gs in the 5'-most G-quartet adopt the syn conformation. These analyses highlight several new aspects of the role of ribose G-quartets on G-quadruplex structure and stability, and demonstrate that the positions of ribose residues are critical for tuning G-quadruplex properties.
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