(15)N NMR Signal Amplification by Reversible Exchange of [(15)N(3)]Ornidazole Antibiotic

通过[(15)N(3)]奥硝唑抗生素的可逆交换实现(15)N NMR信号放大

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Abstract

Hyperpolarization techniques provide a dramatic enhancement of the sensitivity of magnetic resonance spectroscopy and imaging. Signal amplification by reversible exchange in shield enables alignment transfer to heteronuclei (SABRE-SHEATH) is an efficient technique for hyperpolarization of (13)C and (15)N nuclei in various biologically relevant compounds. Nitroimidazole antibiotics are prone to reduction under anaerobic conditions, making them prospective molecular contrast agents for the visualization of hypoxic tumors. In this work, we systematically studied (15)N SABRE-SHEATH hyperpolarization of the ornidazole antibiotic at natural abundance (n.a.) of the (15)N isotope and in the isotopically (15)N(3)-labeled form. Optimization of such experimental conditions as polarization transfer magnetic field, temperature, parahydrogen pressure, and flow rate resulted in average (15)N polarization levels of 9.3 ± 0.5% for n.a. ornidazole and 5.3 ± 0.2% for [(15)N(3)]ornidazole. T(1) polarization decay time of 7.4 min was achieved for the (15)NO(2) group of [(15)N(3)]ornidazole at a clinically relevant 1.4 T magnetic field, allowing for the detection of the (15)N NMR signal more than 20 min after hyperpolarization. DFT calculations of (15)N chemical shifts for ornidazole and plausible intermediates and products of its reduction under hypoxic conditions showed that it should be feasible to discriminate these compounds by using (15)N NMR.

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