On the Role of Ferromagnetic Interactions in Highly Active Mo-Based Catalysts for Ammonia Synthesis

Munarriz, J. (Universidad de Zaragoza) ; Polo, V. (Universidad de Zaragoza) ; Gracia, J.

Resumen: Reactions involving nitrogen fixation and transfer are of great industrial interest. In this regard, unveiling all the physical principles that determine their activity would be enormously beneficial for the rational design of novel catalysts with improved performance. Within this context, this work explores the activity of bulk molybdenum-based transition metal nitrides in ammonia synthesis. Our results highlight that the most active compositions show increasing ferromagnetism in the metal–nitrogen bonds, which constitute the active sites. We observe that the total spin accumulated in the bonds at the active sites is a physically meaningful descriptor to discriminate optimum catalysts. Higher activities are associated with ferromagnetic phases, and the underlying reason is an enhanced overlapping of the electronic wavefunctions; which also make the reaction steps spin-sensitive. These finding provides strong evidence of the general influence of electrons magnetic moment in catalysis, being part of the specific field of spintro-catalysis.

Idioma: Inglés

DOI: 10.1002/cphc.201800633

Año: 2018

Publicado en: CHEMPHYSCHEM 19 (2018), 1-6
ISSN: 1439-4235

Factor impacto JCR: 3.077 (2018)

Categ. JCR: PHYSICS, ATOMIC, MOLECULAR & CHEMICAL rank: 10 / 36 = 0.278 (2018) - Q2 - T1
Categ. JCR: CHEMISTRY, PHYSICAL rank: 63 / 147 = 0.429 (2018) - Q2 - T2

Factor impacto SCIMAGO: 1.08 - Physical and Theoretical Chemistry (Q1) - Atomic and Molecular Physics, and Optics (Q1)

Financiación: info:eu-repo/grantAgreement/ES/DGA/E07
Financiación: info:eu-repo/grantAgreement/ES/MEC/FPU14-06003
Financiación: info:eu-repo/grantAgreement/ES/MINECO/CTQ2015-67366-P

Tipo y forma: Article (Published version)

Área (Departamento): Área Química Física (Dpto. Química Física)