Kovtunov Kirill V, Barskiy Danila A, Shchepin Roman V, Salnikov Oleg G, Prosvirin Igor P, Bukhtiyarov Andrey V, Kovtunova Larisa M, Bukhtiyarov Valerii I, Koptyug Igor V, Chekmenev Eduard Y
Laboratory of Magnetic Resonance Microimaging, International Tomography Center, SB RAS, 3A Institutskaya St., Novosibirsk, 630090, Russia.
Novosibirsk State University, 2 Pirogova St., Novosibirsk, 630090, Russia.
Chemistry. 2016 Nov 7;22(46):16446-16449. doi: 10.1002/chem.201603974. Epub 2016 Oct 10.
A supported metal catalyst was designed, characterized, and tested for aqueous phase heterogeneous hydrogenation of vinyl acetate with parahydrogen to produce C-hyperpolarized ethyl acetate for potential biomedical applications. The Rh/TiO catalyst with a metal loading of 23.2 wt % produced strongly hyperpolarized C-enriched ethyl acetate-1- C detected at 9.4 T. An approximately 14-fold C signal enhancement was detected using circa 50 % parahydrogen gas without taking into account relaxation losses before and after polarization transfer by magnetic field cycling from nascent parahydrogen-derived protons to C nuclei. This first observation of C PHIP-hyperpolarized products over a supported metal catalyst in an aqueous medium opens up new possibilities for production of catalyst-free aqueous solutions of nontoxic hyperpolarized contrast agents for a wide range of biomolecules amenable to the parahydrogen induced polarization by side arm hydrogenation (PHIP-SAH) approach.
设计、表征并测试了一种负载型金属催化剂,用于乙酸乙烯酯与仲氢在水相中的多相氢化反应,以生产用于潜在生物医学应用的碳超极化乙酸乙酯。金属负载量为23.2 wt%的Rh/TiO催化剂产生了在9.4 T下检测到的强超极化碳富集乙酸乙酯-1-碳。在不考虑通过磁场循环从新生仲氢衍生的质子到碳核的极化转移前后的弛豫损失的情况下,使用约50%的仲氢气体检测到约14倍的碳信号增强。在水介质中负载型金属催化剂上首次观察到碳PHIP超极化产物,这为通过侧链氢化(PHIP-SAH)方法生产适用于多种生物分子的无毒超极化造影剂的无催化剂水溶液开辟了新的可能性。