Dataset Information

Highly Selective and Sensitive Detection of PO4 3- Ions in Aqueous Solution by a Luminescent Terbium Metal-Organic Framework.

ABSTRACT: A luminescent terbium metal-organic framework [Tb(HPIA-)(PIA2-)(H2O)2] (Tb-MOF), synthesized by a lanthanide metal ion (Tb3+) and nitric heterocyclic carboxylic acid ligands H2PIA (H2PIA = 5-(1H-pyrazol-3-yl)isophthalic-acid), was structurally characterized as a three-dimensional skeleton structure in which layered coordination frameworks are connected by hydrogen bonds. Based on the antenna effect, Tb-MOF can emit bright green fluorescence under 254 nm excitation, and the fluorescence emission presents excellent durability in aqueous solutions among a wide pH range. Moreover, the structure of Tb-MOF also possesses outstanding thermal stabilities. In some ways, PO4 3- and its derivatives are thought to be a kind of pollutant ion causing series environmental and health problems. The as-synthesized Tb-MOF exhibits prominent selectivity and remarkable sensitivity for detecting PO4 3- as an easy-to-use fluorescent probe with low detection limit, fast response, and wide detection range. Therefore, Tb-MOF has significant applications in the fields of human health and environmental monitoring.

SUBMITTER: Zhao S

PROVIDER: S-EPMC6787892 | biostudies-literature | 2019 Oct

REPOSITORIES: biostudies-literature

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Publications

Highly Selective and Sensitive Detection of PO4 3- Ions in Aqueous Solution by a Luminescent Terbium Metal-Organic Framework.

Zhao Shenglu S Xiao Jiannan J Zheng Tianxiang T Liu Meiying M Wu Haonan H Liu Zhiliang Z

ACS omega 20190923 15

A luminescent terbium metal-organic framework [Tb(HPIA-)(PIA2-)(H2O)2] (Tb-MOF), synthesized by a lanthanide metal ion (Tb3+) and nitric heterocyclic carboxylic acid ligands H2PIA (H2PIA = 5-(1H-pyrazol-3-yl)isophthalic-acid), was structurally characterized as a three-dimensional skeleton structure in which layered coordination frameworks are connected by hydrogen bonds. Based on the antenna effect, Tb-MOF can em ...[more]

PMID: 31616816

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Project description:It has been previously demonstrated that copper-based metal-organic frameworks (MOFs) accelerate formation of the therapeutically active molecule nitric oxide (NO) from S-nitrosothiols (RSNOs). Because RSNOs are naturally present in blood, this function is hypothesized to permit the controlled production of NO through use of MOF-based blood-contacting materials. The practical implementation of MOFs in this application typically requires incorporation within a polymer support, yet this immobilization has been shown to impair the ability of the MOF to interact with the NO-forming RSNO substrate. Here, the water-stable, copper-based MOF H3[(Cu4Cl)3-(BTTri)8] (H3BTTri = 1,3,5-tris(1H-1,2,3-triazol-5-yl)benzene), or Cu-BTTri, was incorporated within the naturally derived polysaccharide chitosan to form membranes that were evaluated for their ability to enhance NO generation from the RSNO S-nitrosoglutathione (GSNO). This is the first report to evaluate MOF-induced NO release from GSNO, the most abundant small-molecule RSNO. At a 20 μM initial GSNO concentration (pH 7.4 phosphate buffered saline, 37 °C), chitosan/Cu-BTTri membranes induced the release of 97 ± 3% of theoretical NO within approximately 4 h, corresponding to a 65-fold increase over the baseline thermal decomposition of GSNO. Furthermore, incorporation of Cu-BTTri within hydrophilic chitosan did not impair the activity of the MOF, unlike earlier efforts using hydrophobic polyurethane or poly(vinyl chloride). The reuse of the membranes continued to enhance NO production from GSNO in subsequent experiments, suggesting the potential for continued use. Additionally, the major organic product of Cu-BTTri-promoted GSNO decomposition was identified as oxidized glutathione via mass spectrometry, confirming prior hypotheses. Structural analysis by pXRD and assessment of copper leaching by ICP-AES indicated that Cu-BTTri retains crystallinity and exhibits no significant degradation following exposure to GSNO. Taken together, these findings provide insight into the function and utility of polymer/Cu-BTTri systems and may support the development of future MOF-based biomaterials.

Project description:The hydration of the alkali metal ions in aqueous solution has been studied by large angle X-ray scattering (LAXS) and double difference infrared spectroscopy (DDIR). The structures of the dimethyl sulfoxide solvated alkali metal ions in solution have been determined to support the studies in aqueous solution. The results of the LAXS and DDIR measurements show that the sodium, potassium, rubidium and cesium ions all are weakly hydrated with only a single shell of water molecules. The smaller lithium ion is more strongly hydrated, most probably with a second hydration shell present. The influence of the rubidium and cesium ions on the water structure was found to be very weak, and it was not possible to quantify this effect in a reliable way due to insufficient separation of the O-D stretching bands of partially deuterated water bound to these metal ions and the O-D stretching bands of the bulk water. Aqueous solutions of sodium, potassium and cesium iodide and cesium and lithium hydroxide have been studied by LAXS and M-O bond distances have been determined fairly accurately except for lithium. However, the number of water molecules binding to the alkali metal ions is very difficult to determine from the LAXS measurements as the number of distances and the temperature factor are strongly correlated. A thorough analysis of M-O bond distances in solid alkali metal compounds with ligands binding through oxygen has been made from available structure databases. There is relatively strong correlation between M-O bond distances and coordination numbers also for the alkali metal ions even though the M-O interactions are weak and the number of complexes of potassium, rubidium and cesium with well-defined coordination geometry is very small. The mean M-O bond distance in the hydrated sodium, potassium, rubidium and cesium ions in aqueous solution have been determined to be 2.43(2), 2.81(1), 2.98(1) and 3.07(1) Å, which corresponds to six-, seven-, eight- and eight-coordination. These coordination numbers are supported by the linear relationship of the hydration enthalpies and the M-O bond distances. This correlation indicates that the hydrated lithium ion is four-coordinate in aqueous solution. New ionic radii are proposed for four- and six-coordinate lithium(I), 0.60 and 0.79 Å, respectively, as well as for five- and six-coordinate sodium(I), 1.02 and 1.07 Å, respectively. The ionic radii for six- and seven-coordinate K(+), 1.38 and 1.46 Å, respectively, and eight-coordinate Rb(+) and Cs(+), 1.64 and 1.73 Å, respectively, are confirmed from previous studies. The M-O bond distances in dimethyl sulfoxide solvated sodium, potassium, rubidium and cesium ions in solution are very similar to those observed in aqueous solution.

Dataset Information

Highly Selective and Sensitive Detection of PO4 3- Ions in Aqueous Solution by a Luminescent Terbium Metal-Organic Framework.

Publications

Highly Selective and Sensitive Detection of PO<sub>4</sub> <sup>3-</sup> Ions in Aqueous Solution by a Luminescent Terbium Metal-Organic Framework.

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