Coloring ultrasensitive MRI with tunable metal–organic frameworks

Yang, Yuqi; Zhang, Yingfeng; Wang, Baolong; Guo, Qianni; Yuan, Yaping; Jiang, Weiping; Shi, Lei; Yang, Minghui; Chen, Shizhen; Lou, Xin; Zhou, Xin

doi:10.1039/d0sc06969h

Cited by 18 publications

(21 citation statements)

References 63 publications

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“…Magnetic resonance can provide both spectroscopic and spatial information simultaneously, thus allowing parallel reading and imaging. Spectrally resolved MRI has been previously realized with various systems based on chemically different diamagnetic compounds 38 – 41 , host-guest interactions 42 , 45 , and lanthanide-induced NMR shifts 43 – 45 . The latter approach offers the advantage to select the NMR shifts without changing the chemical properties, which is particularly useful for in-vivo imaging applications 43 , 44 .…”

Section: Resultsmentioning

confidence: 99%

“…Lanthanides are ideally suited for this purpose, as they provide a range of chemically similar but magnetically different Ln 3+ ions amenable to stable incorporation into organic molecules via coordination 35 , 37 . While distinguishable NMR signals can be obtained from chemically different diamagnetic molecules and formulations 38 – 42 , introducing paramagnetic lanthanides allows for decoupling of the NMR shifts from chemical properties. This principle has been previously used to create chemically nearly identical molecules that could be spectrally resolved with magnetic resonance imaging (MRI) 43 – 45 .…”

Section: Introductionmentioning

confidence: 99%

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Paramagnetic encoding of molecules

et al. 2022

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Contactless digital tags are increasingly penetrating into many areas of human activities. Digitalization of our environment requires an ever growing number of objects to be identified and tracked with machine-readable labels. Molecules offer immense potential to serve for this purpose, but our ability to write, read, and communicate molecular code with current technology remains limited. Here we show that magnetic patterns can be synthetically encoded into stable molecular scaffolds with paramagnetic lanthanide ions to write digital code into molecules and their mixtures. Owing to the directional character of magnetic susceptibility tensors, each sequence of lanthanides built into one molecule produces a unique magnetic outcome. Multiplexing of the encoded molecules provides a high number of codes that grows double-exponentially with the number of available paramagnetic ions. The codes are readable by nuclear magnetic resonance in the radiofrequency (RF) spectrum, analogously to the macroscopic technology of RF identification. A prototype molecular system capable of 16-bit (65,535 codes) encoding is presented. Future optimized systems can conceivably provide 64-bit (~10^19 codes) or higher encoding to cover the labelling needs in drug discovery, anti-counterfeiting and other areas.

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Section: Resultsmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Paramagnetic encoding of molecules

et al. 2022

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“…In another recent study, the capability of 129 Xe hyper-CEST NMR was demonstrated for differentiating a complex mixture containing MOFs as nano-cages in which the latter displayed similar chemical compositions. This was possible by tuning the MOF structure and by encoding multiple false colors for observed Xe chemical shifts 56 . Saturation transfer (ST) techniques are a powerful tool that find an increasing number of applications.…”

Section: Introductionmentioning

confidence: 99%

Hyper-CEST NMR of metal organic polyhedral cages reveals hidden diastereomers with diverse guest exchange kinetics

et al. 2022

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Guest capture and release are important properties of self-assembling nanostructures. Over time, a significant fraction of guests might engage in short-lived states with different symmetry and stereoselectivity and transit frequently between multiple environments, thereby escaping common spectroscopy techniques. Here, we investigate the cavity of an iron-based metal organic polyhedron (Fe-MOP) using spin-hyperpolarized 129Xe Chemical Exchange Saturation Transfer (hyper-CEST) NMR. We report strong signals unknown from previous studies that persist under different perturbations. On-the-fly delivery of hyperpolarized gas yields CEST signatures that reflect different Xe exchange kinetics from multiple environments. Dilute pools with ~ 104-fold lower spin numbers than reported for directly detected hyperpolarized nuclei are readily detected due to efficient guest turnover. The system is further probed by instantaneous and medium timescale perturbations. Computational modeling indicates that these signals originate likely from Xe bound to three Fe-MOP diastereomers (T, C3, S4). The symmetry thus induces steric effects with aperture size changes that tunes selective spin manipulation as it is employed in CEST MRI agents and, potentially, impacts other processes occurring on the millisecond time scale.

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“…Besides, the flexible porosity confers MOFs as candidates of nanocarriers for loading different types of active ingredients involving small molecules, peptides/proteins, or nucleic acids with high loading capacity [ 12 , 13 ]. Furthermore, the unique optical and/or X-ray attenuation abilities of MOFs can be harnessed for molecular imaging, including fluorescence imaging, computed tomography [ 14 ], magnetic resonance imaging [ 15 ], and positron emission tomography [ 16 ]. For therapeutic applications, especially for phototherapy or radiotherapy, photosensitizers and high-Z elements acting as organizing molecular building blocks integrated into the MOFs will augment reactive oxygen species (ROS) production [ 17 , 18 ].…”

Section: Introductionmentioning

confidence: 99%

Two-dimensional metal-organic frameworks: from synthesis to bioapplications

Wang

Jin

et al. 2022

J Nanobiotechnol

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As a typical class of crystalline porous materials, metal–organic framework possesses unique features including versatile functionality, structural and compositional tunability. After being reduced to two-dimension, ultrathin metal-organic framework layers possess more external excellent properties favoring various technological applications. In this review article, the unique structural properties of the ultrathin metal-organic framework nanosheets benefiting from the planar topography were highlighted, involving light transmittance, and electrical conductivity. Moreover, the design strategy and versatile fabrication methodology were summarized covering discussions on their applicability and accessibility, especially for porphyritic metal-organic framework nanosheet. The current achievements in the bioapplications of two-dimensional metal-organic frameworks were presented comprising biocatalysis, biosensor, and theranostic, with an emphasis on reactive oxygen species-based nanomedicine for oncology treatment. Furthermore, current challenges confronting the utilization of two-dimensional metal-organic frameworks and future opportunities in emerging research frontiers were presented. Graphical Abstract

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Coloring ultrasensitive MRI with tunable metal–organic frameworks

Abstract: As one of the most important imaging modalities, magnetic resonance imaging (MRI) still faces relatively low sensitivity to monitor low-abundance molecules. A newly developed technology, hyperpolarized 129Xe magnetic resonance imaging...

Cited by 18 publications

References 63 publications

Paramagnetic encoding of molecules

Paramagnetic encoding of molecules

Hyper-CEST NMR of metal organic polyhedral cages reveals hidden diastereomers with diverse guest exchange kinetics

Two-dimensional metal-organic frameworks: from synthesis to bioapplications

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