Zhao Hai-Qing, Qiu Gui-Hua, Liang Zhen, Li Min-Min, Sun Bin, Qin Liang, Yang Shui-Ping, Chen Wen-Hua, Chen Jin-Xiang
Guangdong Provincial Key Laboratory of New Drug Screening, School of Pharmaceutical Sciences, Southern Medical University, Guangzhou 510515, PR China.
The First Affiliated Hospital of Jinan University, Guangzhou 510515, PR China.
Anal Chim Acta. 2016 May 30;922:55-63. doi: 10.1016/j.aca.2016.03.054. Epub 2016 Apr 7.
Coordination reaction of a known three-dimensional (3D) polymer precursor {Na3[Na9(Cbdcp)6(H2O)18]}n (A, Cbdcp = N-(4-carboxybenzyl)-(3,5-dicarboxyl)pyridinium) with Zn(NO3)2·6H2O in H2O or H2O/DMF at 100 °C and in the presence of aspirin, 5-fluorouracil (5-FU) as modulators, trans-1,2-bis(4-pyridyl)ethylene (bpe) or 1,2-bis(4-pyridyl)ethane (bpea) as ancillary ligands afforded six novel Zn(II)-based metal-organic frameworks (MOFs), that is, {[Zn(Cbdcp)(H2O)3]·H2O}n (1, 1D zigzag chain), {[Zn(HCbdcp)2]·H2O}n (2, 2D sheet), {[Zn(Cbdcp)(bpe)1/2]·2H2O}n (3, 3D polymer), {[Zn(Cbdcp)(bpe)1/2]·2H2O}n (4, 2D network), {[Zn(Cbdcp)(bpea)1/2]·2H2O}n (5, 3D polymer) and {[Zn(Cbdcp)(bpea)1/2]·2H2O}n (6, 2D network). Among them, compound 2 contains aromatic rings, positively charged pyridinium, Zn(2+) cation centers and carboxylic acid groups lined up on the 2D sheet structure with a certain extended surface exposure. The unique structure of 2 facilitates effective association with carboxyfluorescein (FAM) labeled probe single stranded DNA (probe ss-DNA, delineates as P-DNA) to yield a P-DNA@2 system, and leads to fluorescence quenching of FAM via a photoinduced electron transfer process. The P-DNA@2 system is effective and reliable for the detection of human immunodeficiency virus 1 ds-DNA (HIV ds-DNA) sequences and capable of distinguishing complementary HIV ds-DNA from mismatched target sequences with the detection limit as low as 10 pM (S/N = 3).
已知的三维(3D)聚合物前驱体{Na3[Na9(Cbdcp)6(H2O)18]}n(A,Cbdcp = N-(4-羧基苄基)-(3,5-二羧基)吡啶鎓)与Zn(NO3)2·6H2O在100°C的水或水/二甲基甲酰胺(DMF)中,在阿司匹林、5-氟尿嘧啶(5-FU)作为调节剂,反式-1,2-双(4-吡啶基)乙烯(bpe)或1,2-双(4-吡啶基)乙烷(bpea)作为辅助配体的存在下发生配位反应,得到了六种新型的基于Zn(II)的金属有机框架(MOF),即{[Zn(Cbdcp)(H2O)3]·H2O}n(1,一维锯齿链),{[Zn(HCbdcp)2]·H2O}n(2,二维片层),{[Zn(Cbdcp)(bpe)1/2]·2H2O}n(3,三维聚合物),{[Zn(Cbdcp)(bpe)1/2]·2H2O}n(4,二维网络),{[Zn(Cbdcp)(bpea)1/2]·2H2O}n(5,三维聚合物)和{[Zn(Cbdcp)(bpea)1/2]·2H2O}n(6,二维网络)。其中,化合物2在二维片层结构上含有芳香环、带正电荷的吡啶鎓、Zn(2+)阳离子中心和羧酸基团,具有一定的扩展表面暴露。2的独特结构有利于与羧基荧光素(FAM)标记的探针单链DNA(探针ss-DNA,记为P-DNA)有效结合,形成P-DNA@2体系,并通过光诱导电子转移过程导致FAM荧光猝灭。P-DNA@2体系对人免疫缺陷病毒1双链DNA(HIV ds-DNA)序列的检测有效且可靠,能够区分互补的HIV ds-DNA与错配的靶序列,检测限低至10 pM(S/N = 3)。