Synthesis and Fluorescence Sensing for Nitro Explosives and Pesticides of Two Cd-Coordination Polymers
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PROVIDER: S-EPMC10600892 | biostudies-literature | 2023 Oct
REPOSITORIES: biostudies-literature
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Project description:By rational assembly of polytorsional-amide [N,N'-bis(4-methylenepyridin-4-yl)-1,4-naphthalene dicarboxamide (L)] and polytorsional-carboxylates [H2ADI = adipic acid, H2PIM = pimelic acid, H2SUB = suberic acid], three new Cd-based coordination polymers (CPs) C30H30CdN4O7 (1), C31H32CdN4O7 (2) and C31.03H30.55CdCl0.24N4O5.52 (3) were successfully synthesized. CPs 1-2 and 3 are 2D networks and a 3D framework, which all display 3,5-connected topologies with different structural details. The effects of carboxylates with different carbon chains on the structure of the complexes were studied. Fluorescence experiments show that CPs 1-3 have good multi-functional sensing ability for metal cations (Fe3+), anions (MnO4 -, CrO4 2-, Cr2O7 2-) and organochlorine pesticides (2,6-dichloro-4-nitroamine) with good anti-interference and recyclable characteristics. The possible sensing mechanism is also investigated in detail.
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Project description:In the past decades, porous coordination polymers (PCPs) based fluorescent (FL) sensors have received intense attention due to their promising applications. In this work, a soluble Zn-PCP is presented as a sensitive probe towards explosive molecules, chromate, and dichromate ions. In former reports, PCP sensors were usually ground into fine powders and then dispersed in solvents to form FL emulsion for sensing applications. However, their insoluble characters would cause the sensing accuracy which is prone to interference from environmental effects. While in this work, the as-made PCP could be directly soluble in organic solvents to form a clear solution with bright blue emission, representing the first soluble PCP based fluorescence sensor to probe explosive molecules under a homogeneous environment. Moreover, the FL PCP solution also shows sensitive detection behaviors towards the toxic anions of CrO42- and Cr2O72-, which exhibit a good linear relationship between the fluorescence intensity of Zn-PCP and the concentrations of both analytes. This work provides a reference for designing task-specific PCP sensors utilized under a homogeneous environment.
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Project description:Three couples of coordination polymers (CPs), namely, [Co((R/S)-Hcna)2] n (1-D/L), [Cd6((1R,2R/1S,2S)-cpba)4(phen)6(H2O)3] n (2-D/L) and [Cd2((1R,2R/1S,2S)-Hcpba)2(phen)2] n (3-D/L) {(R/S)-H2cna = (R/S)-6-(1-carboxyethoxy)-2-naphthoic acid, (1R,2R/1S,2S)-H3cpba = (1R,2R/1S,2S)-2,2'-((5-carboxy-1,3-phenylene)bis(oxy))dipropionic acid, phen = 1,10-phenanthroline} are successfully synthesized under hydrothermal conditions. Structural analysis shows that CP 1 has a 3D 3,6-c net structure with a point symbol of (4·62)2(42·610·83). CPs 2 and 3 are obtained under very similar reaction conditions except using different solvent ratios. The presence of the planar chelating ligand phen in CPs 2 and 3 limited the spatial growth of the structure, resulting in the formation of different 1D structures. All CPs crystallized in the chiral space group P21, CPs 1-3 are all SHG active. Their luminescence sensing activities for organics such as antibiotics, pesticides and nitro aromatics are also investigated. The results showed that CP 1 can effectively identify trace amounts of nitrofurans (NFs) and CP 3 has obvious recognition ability toward nitrofurans (NFs) and nitroimidazoles (NMs). Both CPs 1 and 3 could selectively detect 2,6-dichloro-4-nitroaniline (DCN). The luminescence of CPs 1 and 3 can also be quenched by (D/L)-4-nitrophenylalanine ((D/L)-NPA) and (1R,2R/1S,2S)-2-amino-1-(4-nitrophenyl)propane-1,3-diol ((1R,2R/1S,2S)-ANPO).
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Project description:Ratiometric fluorescent sensing based on dual-emitting fluorescent coordination polymers (FL-CPs) has attracted intense attention due to their sensing accuracy and easy visualization when compared with sensing relying solely on monochromatic FL-CPs. In this work, a series of rare-earth metal-based CPs, formuled as [(CH3)2NH2][Ln(bpdc)2] (Ln3+ = Y3+, Eu3+ and Tb3+, H2bpdc = biphenyl-4,4'-dicarboxylic acid), are presented, which show dual emission aroused from the Ln3+ ions and the inefficient intermolecular energy transfer from ligands to Ln3+ metals. For clarity, the as-made Ln-CPs are named Eu-bpdc, Tb-bpdc, and Y-bpdc based on the corresponding Ln3+. Notably, Eu-bpdc, presented as an example, could be used as FL sensing material ratiometric to Fe3+ ions. The ratio of FL intensity of Eu3+ ions to bpdc2- ligands (I415/I615) showed a good linear relationship with the concentrations of Fe3+ ions. Moreover, the detection process could be visibly monitored through a change from purple to blue when Eu-bpdc was used as an FL proble. This work provides a good example for exploring visibly ratiometric sensors based on FL-CPs.
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Project description:The high sensitivity of silole- and silafluorene-containing polymers for detecting organic nitro, nitrate, and nitramine explosives cannot be solely attributed to favorable analyte-polymer hydrophobic interactions and amplified fluorescence quenching due to delocalization along the polymer chain. The Lewis acidity of silicon in conjugated poly(silafluorene-vinylene)s is shown to be important. This was established by examining the (29)Si NMR chemical shifts (Delta) for the model trimer fragment of the polymer CH(3)-silafluorene-(trans-C(2)H(2))-silafluorene-(trans-C(2)H(2))-silafluorene-CH(3). The peripheral and central silicon resonances are up-field from a TMS reference at -9.50 and -18.9 ppm, respectively. Both resonances shift down-field in the presence of donor analytes and the observed shifts (0 to 1 ppm) correlate with the basicity of a variety of added Lewis bases, including TNT. The most basic analyte studied was acetonitrile and an association constant (K(a)) of 0.12 M(-1) was calculated its binding to the peripheral silicon centers using the Scatchard method. Spin-lattice relaxation times (T(1)) of 5.86(3) and 4.83(4) s were measured for the methyl protons of acetonitrile in benzene-d(6) at 20 degrees C in the absence and presence of the silafluorene trimer, respectively. The significant change in T(1) values further supports a binding event between acetonitrile and the silafluorene trimer. These studies as well as significant changes and shifts observed in the characteristic UV-Vis absorption of the silafluorene group support an important role for the Lewis acid character of Si in polymer sensors that incorporate strained silacycles. The nitro groups of high explosives may act as weak Lewis-base donors to silacycles. This provides a donor-acceptor interaction that may be crucial for orienting the explosive analyte in the polymer film to provide an efficient pathway for inner-sphere electron transfer during the electron-transfer quenching process.
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