Theoretical Views on Catalytic Reaction Pathways for Nitrogen Fixation by Dinitrogen-Bridging Dimolybdenum Complexes

Egi, Akihito; Tanaka, Hiromasa; Yoshizawa, Kazunari

doi:10.5059/yukigoseikyokaishi.79.1041

Cited by 1 publication

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“…Here, we focus on single molybdenum centers to provide some initial systematic theoretical investigation. Different models have recently been developed to elucidate the activity of terminal monometallic N 2 complexes as opposed to bridging bimetallic N 2 complexes. ,− To these ends, we extend our previous theoretical study of the Mo atoms and ions (0, ±1, ±2) + N 2 reaction in two different directions. First, we explore the negatively charged single metal centers, which have recently been found to have superior performance for other significant chemical processes, such us methane to methanol transformation. , Second, we add ligands in a systematic manner and, finally, study the effects of various ligands for saturated complexes.…”

Section: Introductionmentioning

confidence: 91%

Electronic Structure and Ligand Effects on the Activation and Cleavage of N₂ on a Molybdenum Center

White,

Claveau,

Miliordos

et al. 2024

J. Phys. Chem. A

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Dinitrogen fixation under ambient conditions remains a challenge in the field of catalytic chemistry due to the inertness of N2. Nitrogenases and heterogeneous solid catalysts have displayed remarkable performance in the catalytic conversion of dinitrogen to ammonia. By introduction of molybdenum centers in molecular complexes, one of the most azophilic metals of the transitional metal series, moderate ammonia yields have been attained. Here, we present a combined multiconfigurational/density functional theory study that addresses how ligand fields of different strengths affect the binding and activation of dinitrogen on molybdenum atoms. First, we explored with MRCI computations the diatomic Mo–N and triatomic Mo–N2 molecular systems. Then, we performed a systematic examination on the stabilization effects introduced by external NH3 ligands, before we explore model neutral and charged complexes with different types of ligands (H2O, NH3, and PH3) and their consequences on the N2 binding and activation.

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Section: Introductionmentioning

confidence: 91%

Electronic Structure and Ligand Effects on the Activation and Cleavage of N₂ on a Molybdenum Center

White,

Claveau,

Miliordos

et al. 2024

J. Phys. Chem. A

View full text Add to dashboard Cite

show abstract

Theoretical Views on Catalytic Reaction Pathways for Nitrogen Fixation by Dinitrogen-Bridging Dimolybdenum Complexes

Cited by 1 publication

References 34 publications

Electronic Structure and Ligand Effects on the Activation and Cleavage of N₂ on a Molybdenum Center

Electronic Structure and Ligand Effects on the Activation and Cleavage of N₂ on a Molybdenum Center

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Theoretical Views on Catalytic Reaction Pathways for Nitrogen Fixation by Dinitrogen-Bridging Dimolybdenum Complexes

Cited by 1 publication

References 34 publications

Electronic Structure and Ligand Effects on the Activation and Cleavage of N2 on a Molybdenum Center

Electronic Structure and Ligand Effects on the Activation and Cleavage of N2 on a Molybdenum Center

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Electronic Structure and Ligand Effects on the Activation and Cleavage of N₂ on a Molybdenum Center

Electronic Structure and Ligand Effects on the Activation and Cleavage of N₂ on a Molybdenum Center