Sanofi Germany, R&D, Integrated Drug Discovery, Industriepark Höchst, 65926, Frankfurt am Main, Germany.
Department Chemie, Johannes Gutenberg-Universität Mainz, Duesbergweg 10-14, 55128, Mainz, Germany.
Angew Chem Int Ed Engl. 2023 Jun 12;62(24):e202301512. doi: 10.1002/anie.202301512. Epub 2023 May 4.
We have studied the highly selective homogeneous iridium-catalyzed hydrogen isotope exchange (HIE) with deuterium or tritium gas as an isotope source in water and buffers. With an improved water-soluble Kerr-type catalyst, we have achieved the first insight into applying HIE reactions in aqueous media with varying pH. Density functional theory (DFT) calculations gave consistent insights in the calculated energies of transition states and coordination complexes, further explaining the observed reactivity and guidance on the scope and limitations for HIE reactions in water. Finally, we successfully adapted these findings to tritium chemistry.
我们研究了在水中和缓冲液中使用氘气或氚气作为同位素源的高选择性均相铱催化氢同位素交换（HIE）。通过改进的水溶性 Kerr 型催化剂，我们首次深入了解了在不同 pH 值的水介质中应用 HIE 反应。密度泛函理论（DFT）计算在计算过渡态和配位络合物的能量方面提供了一致的见解，进一步解释了观察到的反应性，并指导了在水中进行 HIE 反应的范围和限制。最后，我们成功地将这些发现应用于氚化学。
