2025-07-21 スイス連邦工科大学ローザンヌ校(EPFL)
<関連情報>
- https://actu.epfl.ch/news/uranium-based-catalyst-turns-air-nitrogen-into-amm/
- https://www.nature.com/articles/s41557-025-01867-z
ウラン錯体を介したサイドオン結合二窒素のアンモニアへの触媒的・化学量論的段階的変換 Catalytic and stoichiometric stepwise conversion of side-on bound dinitrogen to ammonia mediated by a uranium complex
Mikhail S. Batov,Heather T. Partlow,Lucile Chatelain,John A. Seed,Rosario Scopelliti,Ivica Zivkovic,Ralph W. Adams,Stephen T. Liddle & Marinella Mazzanti
Nature Chemistry Published:16 July 2025
DOI:https://doi.org/10.1038/s41557-025-01867-z

Abstract
The well-defined catalytic conversion of dinitrogen (N2) to ammonia (NH3) by molecular complexes is of fundamental interest and important for providing an atomic-level understanding of reactivity that can be related to industrial and biological nitrogen-fixation processes. Molecular catalytic N2 to NH3 conversion currently involves the reduction and protonation of terminal or bridging end-on bound metal–N2 complexes. However, catalytic N2 to NH3 conversion by side-on bound metal–N2 molecular complexes is relevant to both the industrial and biological nitrogen-fixation processes. Here, using a uranium triamidoamine complex, we report catalytic N2 to NH3 conversion involving side-on bound N2 binding. Stoichiometric reactions reveal stepwise reduction of N2 from free N2 to bridging side-on bound forms and subsequently to bridging nitrides, uniquely accessing four different states of side-on bound N2 for the same molecular system. This reveals the roles of N2, N22−, N23−, N24− and N3− in the catalytic conversion of N2 to NH3 when involving side-on bridging N2.


