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Hyperpolarized Xe NMR signal advancement by metal-organic framework entrapment in aqueous solution.

ABSTRACT: We report hyperpolarized Xe signal advancement by metal-organic framework (MOF) entrapment (Hyper-SAME) in aqueous solution. The ¹²⁹Xe NMR signal is drastically promoted by entrapping the Xe into the pores of MOFs. The chemical shift of entrapped ¹²⁹Xe is clearly distinguishable from that of free ¹²⁹Xe in water, due to the surface and pore environment of MOFs. The influences from the crystal size of MOFs and their concentration in water are studied. A zinc imidazole MOF, zeolitic imidazole framework-8 (ZIF-8), with particle size of 110 nm at a concentration of 100 mg/mL, was used to give an NMR signal with intensity four times that of free ¹²⁹Xe in water. Additionally, Hyper-SAME is compatible with hyperpolarized ¹²⁹Xe chemical exchange saturation transfer. The ¹²⁹Xe NMR signal can be amplified further by combining the two techniques. More importantly, Hyper-SAME provides a way to make detection of hyperpolarized ¹²⁹Xe in aqueous solution convenient and broadens the application area of MOFs.

SUBMITTER: Zeng Q

PROVIDER: S-EPMC7395552 | biostudies-literature | 2020 Jul

REPOSITORIES: biostudies-literature

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Hyperpolarized Xe NMR signal advancement by metal-organic framework entrapment in aqueous solution.

Zeng Qingbin Q Bie Binglin B Guo Qianni Q Yuan Yaping Y Han Qi Q Han Xiaocang X Chen Mingwei M Zhang Xu X Yang Yunhuang Y Liu Maili M Liu Pan P Deng Hexiang H Zhou Xin X

Proceedings of the National Academy of Sciences of the United States of America 20200713 30

We report hyperpolarized Xe signal advancement by metal-organic framework (MOF) entrapment (Hyper-SAME) in aqueous solution. The 129Xe NMR signal is drastically promoted by entrapping the Xe into the pores of MOFs. The chemical shift of entrapped 129Xe is clearly distinguishable from that of free 129Xe in water, due to the surface and pore environment of MOFs. The influences from the crystal size of MOFs and their concentration in water are studied. A zinc imidaz ...[more]

PMID: 32661173

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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.

Dataset Information

Hyperpolarized Xe NMR signal advancement by metal-organic framework entrapment in aqueous solution.

Publications

Hyperpolarized Xe NMR signal advancement by metal-organic framework entrapment in aqueous solution.

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