Proton-Coupled Electron Transfer in the Oxidation of Guanosine Monophosphate by Ru(bpy)33+

被引：2
|
作者：
Murphy, Christine Fecenko [1 ,2 ]
Dongare, Prateek [1 ]
Weatherly, Stephanie C. [1 ]
Gagliardi, Christopher J. [1 ]
Thorp, H. Holden [1 ,3 ]
Meyer, Thomas J. [1 ]
机构：
[1] Univ N Carolina, Dept Chem, Chapel Hill, NC 27599 USA
[2] Princeton Univ, Grad Sch, Princeton, NJ 08540 USA
[3] Washington Univ, Off Provost, St Louis, MO USA
来源：
JOURNAL OF PHYSICAL CHEMISTRY C | 2018年 / 122卷 / 43期
基金：
美国国家科学基金会;
关键词：
RADICAL-CATION DEPROTONATION; GUANINE OXIDATION; ELECTROCATALYTIC OXIDATION; DUPLEX DNA; METAL-COMPLEXES; G-QUADRUPLEX; ISOTOPE; PHENOLS; MECHANISM; NUCLEOBASES;
D O I：
10.1021/acs.jpcc.8b08382
中图分类号：
O64 [物理化学（理论化学）、化学物理学];
学科分类号：
070304 ; 081704 ;
摘要：
Oxidation of guanine by the outer-sphere metal complex oxidant Ru(bpy)(3)(3+) (bpy is 2,2'-bipyridine) has been explored in deoxyguanosine-5'-monophosphate with the added buffers succinic acid/succinate Hsuc/suc(-center dot) (pK(a) = 5.6), H2PO4-/HPO42- (pK(a) = 7.2), and Tris [(HOCH2)(3)CNH3+/(HOCH2)(3)CNH2] (pK(a) = 8.1) at 23 +/- 2 degrees C. Over an extended range of buffer concentrations and ratios, there is clear evidence for the mechanistic importance of pathways involving concerted electron proton transfer. In this pathway, proton transfer to the base form of the buffer occurs in concert with electron transfer to the oxidant, Ru(bpy)(3)(3+).
引用
收藏
页码：24830 / 24837
页数：8
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