TRUFA · Transition metal-Uranium FLPs for the cooperative Activation of dinitrogen

Transition metal-Uranium FLPs for the cooperative Activation of dinitrogen

The conversion of atmospheric dinitrogen into ammonia consumes around 1% of the global energy demand. Milder efficient nitrogen fixation methodologies remain one of the greatest challenges in modern chemistry. Frustrated Lewis Pairs (FLPs) excel to activate small molecules, yet their involvement in N2 chemistry remains an unmet challenge. Inspired by the independent 2017 reports of Szymczak and Simonneau on the activation of transition metal dinitrogen complexes by Lewis acids, and taking into consideration the rich chemistry of low-valent uranium towards N2, this project envisioned the cooperative activation and functionalization of N2 by electron rich transition metals and electrophilic U(III) complexes. Importantly, at the time of the project, there was only one report displaying cooperative N2 activation by a transition metal and uranium (Cummins, 1998). Besides this, end-on coordination of N2 to uranium was only known for a couple of examples (Evans 2003, Liddle 2019). In addition, transition metal-catalysis is a key area of industrial interest: exploring new avenues to improve the performance of catalysts remains a pivotal aspect to enable more efficient and sustainable transformations.

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