| Acquired immune deficiency syndrome (Aids) and ebola hemorrhagic fever (EHF) are two kinds of dangerous diseases that Aids is caused by Human Immunodeficiency Virus (HTV) while EHF is induced by Ebola Virus (EBOV). Sudan virus (SUDV) is more harmful as one kind of EBOV. Up to date, there is no effective drug or vaccine for these two diseases. Therefore, early diagnosis of virus is significant for the discovery and isolation of the patients.Useful methods detecting virus in clinical trials are often laborious and/or require high-cost instrumentation. Metal organic frameworks (MOFs), a new kind of virus nucleic acid molecule detection reagent, have attracted widespread attention due to their low price and excellent performance with rapid response, high efficiency, sensitivity and simple operation. All these make them as potential sensing agents for clinical detection of virus nucleic acid molecule for diagnosis of related diseases. However, few MOFs have been explored for the detection of DNA or RNA because of their poor water stability.In recent years, we have been keenly interested in coordination compounds based on quaternized-carboxylate ligands. We have shown that a diverse framework materials assembled from these ligands exhibited high water stability, as well as potent DNA binding activity. In this thesis, we synthesized three types of quaternized carboxylates, and their corresponding 11 water stable metal organic frameworks. We also investigated activities from some of them for the detection of HIV-1 dsDNA and SUDV RNA. The obtained results are summarized below.Part 1:We designed two new zwitterionic tricarboxylic ligands of HsCmdcpBr (H3CmdcpBr = N-carboxymethyl-(3,5-dicarboxyl) pyridinium bromide) and H3CbdcpBr (H3CbdcpBr = N-(4-carboxybenzyl)-(3,5-dicarboxyl) pyridinium bromide). Further reaction with lanthanide Ln(III) ions, we got five water stable compounds [Ln4(Cmdcp)6(H2O)9]n (Ln = La (1), Ce (2), Pr (3), Nd (4) and [La2(Cbdcp)3(H20)10]n (5). Compounds 1-5 show good water stability. All these compounds were characterized by IR, elemental analyses and single crystal X-ray crystallography. Among them, compound 1-4 have same structure that contain 3D framework with a hexagonal-shaped one-dimensional (ID) channels with side length 9.6 A. While compound 5 shows a 2D structure. As comparison, we selected two La-based MOFs, that is 1 with 3D structure and 5 with 2D structure, as sensing platform for HIV-1 dsDNA and SUDV RNA sequences. For HIV-1 dsDNA, the quenching efficiencies (Qe) of compound 1 and 5 to P-DNA are 63.5% and 56.3% and the recover efficiencies (Re) are 0.5 and 0.58, the recovery times are 48 min and 30 min, the detection limits are 223 pM and 89 pM. For SUDV RNA sequences with 20 bases, the quenching efficiencies (Qe) to P-DNA are 70.3% and 57.2%, the recover efficiencies (Re) are 0.62 and 0.78, the recovery times are 48 min and 35 min, the detection limits are 112 pM and 67 pM. With the target SUDV RNA sequences increased to 30 or 40 bases, the detection ability of compound 1 and 5 have become weakened. These results indicate that both compounds 1 and 5 can be used as specifitic detection of HIV-1 dsDNA and SUDV RNA sequences, but with low RE values.Part 2:To seek MOFs with better detection performance, we got a new MOF [Cu3(Cmdcp)2(dps)4(H2O)4(SO4)]n (6) from the reaction of H3CmdcpBr with Cu(II) and 4,4’-dipyridyl sulfide (dps). MOF 6 was characterized by IR, elemental analyses and single crystal X-ray crystallography. It has Kagome cross section that hexagonal-shaped one-dimensional (ID) channels with approximately 16.6 × 9.7 A2 in dimension. It has good water stability and thermal stability. For its detection of HIV-1 dsDNA, the quenching efficiency (QE) to P-DNA is 65.3%, the recover efficiency (Re) is 0.91, the recovery time is 90 min and the detection limits is 196 pM. The data for SUDV RNA is 76.3%,2.27 30 min and 73 pM, respectively. MOF 6 can efficiently detect the target SUDV RNA sequences with up to 80 bases..Part 3:Based on the previous two parts, we designed a new zwitterionic tricarboxylic acid ligand, HsCdcbpBr (H3CdcbpBr= 3-Carboxy-l-(3,5-dicarboxy-benzyl)-pyridinium bromide), with different auxiliary ligands, we have synthesized its five water stable copper Cu (II) compounds [Cu(Cdcbp)(H2O)4]n (7), [Cu(Cdcbp)(phen)2]n (8), [Cu(Cdcbp)(dps)]n (9), [Cu(Cdcbp)(bpe)]n (10) and [Cu(Cdcbp)(bpea)]n (11). All these compounds were characterized by IR, elemental analyses and single crystal X-ray crystallography. Among them, compound 7 and 9 have ID chain structure while 8 is a mononuclear compound.10 and 11 have same structure with 3D framework. We choose 11 that has higher yield used for detection experiment. When detecting HIV-1 dsDNA, the quenching efficiency (QE) to P-DNA is 65.1%, the recover efficiency (RE) is 0.98, the recovery time is 34 min and the detection limits is 81 pM. The data for SUDV RNA is 83.3%,2.4,23 min and 31 pM, respective. Further research shows that the compound 11 can efficiently detect the target SUDV RNA sequences with up to 80 bases. |
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