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The formed tetravalent Mo was found to be capable of inducing better electronic interactions between the surface nitrogen species and the Fe metal groups, thus improving the FE.
Ambient atomic orbitals series#
To overcome the low faradaic efficiency (FE) of single Mo or Fe based electrocatalysts in nitrogen reduction reactions (NRR) due to the competition from the hydrogen evolution reaction (HER), a series of bimetallic MoFe compound catalysts were prepared under an NH3 atmosphere through a facile precipitation-pyrolysis method. The in situ synthesized platinum nitride clusters, typically Pt3N7+, induce highly active N site for hydrogen anchoring, enabling a cost-effective hydrotreating process for ammonia synthesis. Furthermore, by reacting the PtnNm+ clusters with H2, we observed hydrogenation products of both even- and odd-hydrogen species indicative of ammonia release. A key intermediate containing a bridged N2 of binding with two Pt clusters facilitates N2 activation with significantly enhanced interactions between the d orbitals of Pt and the antibonding π*-orbitals of N2. We illustrate that a chain reaction path within dual cluster cooperation, especially via a “3+2” mode, is beneficial to N≡N triple bond dissociation, embodying efficient synergistic catalysis. The reactivity of Pt3+ is found to be substantially higher than that of other clusters, and the formed Pt3N7+ shows prominent mass abundance among the odd-nitrogen products. Here, we report a breakthrough in efficient dinitrogen cleavage by employing small Ptn+ (n=1-4) clusters and convenient plasma assistance. The activation and reduction of N2 to produce ammonia under mild conditions is of great interest, but challenges remain.