Graduate School of Science, Nagoya University, Chikusa, Nagoya, 464-8602, Japan.
Sci Rep. 2017 May 16;7(1):1586. doi: 10.1038/s41598-017-01645-z.
Amides are ubiquitous and abundant in nature and our society, but are very stable and reluctant to salt-free, catalytic chemical transformations. Through the activation of a "sterically confined bipyridine-ruthenium (Ru) framework (molecularly well-designed site to confine adsorbed H in)" of a precatalyst, catalytic hydrogenation of formamides through polyamide is achieved under a wide range of reaction conditions. Both C=O bond and C-N bond cleavage of a lactam became also possible using a single precatalyst. That is, catalyst diversity is induced by activation and stepwise multiple hydrogenation of a single precatalyst when the conditions are varied. The versatile catalysts have different structures and different resting states for multifaceted amide hydrogenation, but the common structure produced upon reaction with H, which catalyzes hydrogenation, seems to be "H-Ru-N-H."
酰胺在自然界和我们的社会中无处不在且含量丰富，但它们非常稳定，不易进行无盐、催化的化学转化。通过对前催化剂中“空间受限的联吡啶-钌（Ru）框架（分子设计的位点，用于限制吸附的 H）”的活化，酰胺在广泛的反应条件下通过聚酰胺实现催化氢化。使用单个前催化剂也可以实现内酰胺的 C=O 键和 C-N 键的断裂。也就是说，当条件发生变化时，通过单个前催化剂的活化和分步多步加氢，诱导出催化剂的多样性。多功能催化剂具有不同的结构和不同的酰胺加氢的休眠状态，但与 H 反应生成的共同结构似乎是“H-Ru-N-H”。
