Rhodium nanocatalysts and hyperpolarization - synthesis and production of biomedical contrast agents
Final Report Abstract
Nuclear magnetic resonance (NMR) is an intrinsically insensitive phenomenon. Hyperpolarization methods have been developed to amplify signals by several orders of magnitude. One of these is based on para-hydrogen, which is a spin isomer of hydrogen gas. This can be used to carry out hydrogenations in solvents using a catalyst. Over the past few years, the use of para-hydrogen for signal amplification of metabolites has moved into the focus, as it promises to be used as a contrast agent for biomedical imaging. The advantage of this method is that it can increase the signal of metabolic products in just a few seconds. In the course of the project, possibilities should be investigated to produce nanocatalysts with which metabolites can be efficiently hyperpolarized and which can be made easily separable so that a purified solution can be obtained to carry out metabolic studies. Ligands, forms and immobilization strategies were to be analyzed. At the beginning of the project, deuterated ligands were produced that showed positive effects on polarization. However, as it was difficult to polarize concentrations larger than the single-digit millimolar range, alternative separation methods for homogeneous catalysts were investigated. In the course of this, a process was developed in which catalysts can be precipitated and filtered off and injection solutions with only micromolar metal concentrations are obtained that show more than 95% cell viability. This was then used to carry out cell studies, in particular to investigate pyruvatelactate metabolism. Finally, we were able to record the first successful tumor images with para-hydrogen-generated metabolites due to the developed purification process.
Publications
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Signal-enhanced real-time magnetic resonance of enzymatic reactions at millitesla fields. Chemical Science, 12(1), 314-319.
Korchak, Sergey; Jagtap, Anil P. & Glöggler, Stefan
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Spontaneous Enhancement of Magnetic Resonance Signals Using a RASER. Angewandte Chemie, 133(38), 21152-21158.
Korchak, Sergey; Kaltschnee, Lukas; Dervisoglu, Riza; Andreas, Loren; Griesinger, Christian & Glöggler, Stefan
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A Field‐Independent Method for the Rapid Generation of Hyperpolarized [1‐13C]Pyruvate in Clean Water Solutions for Biomedical Applications. Angewandte Chemie International Edition, 61(34).
Mamone, Salvatore; Jagtap, Anil P.; Korchak, Sergey; Ding, Yonghong; Sternkopf, Sonja & Glöggler, Stefan
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Metabolic Tumor Imaging with Rapidly Signal‐Enhanced 1‐13C‐Pyruvate‐d3. ChemPhysChem, 24(2).
Hune, Theresa; Mamone, Salvatore; Schroeder, Henning; Jagtap, Anil P.; Sternkopf, Sonja; Stevanato, Gabriele; Korchak, Sergey; Fokken, Claudia; Müller, Christoph A.; Schmidt, Andreas B.; Becker, Dorothea & Glöggler, Stefan
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Rapidly Signal‐enhanced Metabolites for Atomic Scale Monitoring of Living Cells with Magnetic Resonance. Chemistry–Methods, 2(7).
Ding, Yonghong; Korchak, Sergey; Mamone, Salvatore; Jagtap, Anil P.; Stevanato, Gabriele; Sternkopf, Sonja; Moll, Denis; Schroeder, Henning; Becker, Stefan; Fischer, André; Gerhardt, Ellen; Outeiro, Tiago F.; Opazo, Felipe; Griesinger, Christian & Glöggler, Stefan
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Real-time cell metabolism assessed repeatedly on the same cells via para-hydrogen induced polarization. Chemical Science, 14(28), 7642-7647.
Ding, Yonghong; Stevanato, Gabriele; von Bonin, Frederike; Kube, Dieter & Glöggler, Stefan
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Real-Time Pyruvate Chemical Conversion Monitoring Enabled by PHIP. Journal of the American Chemical Society, 145(10), 5864-5871.
Stevanato, Gabriele; Ding, Yonghong; Mamone, Salvatore; Jagtap, Anil P.; Korchak, Sergey & Glöggler, Stefan
