Development of Group4 Transition Metal Polyhydride Complexes for Dinitrogen Activation

我们成功地创造了一种新型的多金属多氢化钛化合物，该化合物可以在环境温度和压力下裂解二氮键并形成氮-氢键，而无需额外的还原剂或质子源。该多氢化钛化合物可以通过消除H2产生足够的电子来断裂氮三键，这是每损失一个H2单元两个电子的来源，并用作氨前体的氢源。此外，金属中心可能通过生物固氮和哈伯-博施过程中的协同效应增强N2活化。在一个反应中观察到N2活化、键断裂和N-H键形成步骤是前所未有的。这一结果为寻找温和的二氮还原催化剂提供了希望。

We successfully created a novel multi-metallic titanium polyhydride compound that can cleave the dinitrogen bond and form nitrogen-hydrogen bond at ambient temperature and pressure without additional reducing agents or proton sources.The titanium polyhydride compound can generate sufficient electrons to break nitrogen triple bonds by elimination of H2, which is a source of two electrons for each H2 unit lost, and act as a hydrogen source for ammonia precursors. Furthermore, the metal centers might enhance N2 activation through cooperative effects seen in biological nitrogen fixation and the Haber-Bosch process. This is unprecedented to observe N2 activation, bond cleavage and N-H bond formation steps in one reaction. This result offers hope in the search for mild dinitrogen reduction catalysts.