Catalytic activation of N2O on promoted NiO based materials: Valorization by oxidative dehydrogenation of ethane

[EN] N2O-assisted Oxidative Dehydrogenation (ODH) of ethane is an interesting way of simultaneously obtaining a highly valuable raw material (ethylene) and the functionalization of a greenhouse gas (N2O). Unfortunately, over most of the catalytic systems, this reaction presents two main drawbacks: i...

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Detalhes bibliográficos
Autores: Sánchez-García, G., Pérez-Calvo, A., Sánchez-Tovar, R., Dejoz, A.M., Solsona, B., Moreno-Torralbo, Beatriz Maria, Concepción Heydorn, Patricia|||0000-0003-2058-3103, López Nieto, José Manuel|||0000-0002-6960-3219
Formato: artículo
Fecha de publicación:2025
País:España
Recursos:Universitat Politècnica de València (UPV)
Repositorio:RiuNet. Repositorio Institucional de la Universitat Politécnica de Valéncia
Idioma:inglés
OAI Identifier:oai:riunet.upv.es:10251/224429
Acesso em linha:https://riunet.upv.es/handle/10251/224429
Access Level:acceso abierto
Palavra-chave:N2O
Oxidative dehydrogenation of ethane
Catalysis vs electrochemistry
Niobium
NiO
Temperature programmed reaction of ethane/N2O
Descrição
Resumo:[EN] N2O-assisted Oxidative Dehydrogenation (ODH) of ethane is an interesting way of simultaneously obtaining a highly valuable raw material (ethylene) and the functionalization of a greenhouse gas (N2O). Unfortunately, over most of the catalytic systems, this reaction presents two main drawbacks: i) high yields to ethylene have hardly been reported; and ii) the catalytic activity highly decreases when replacing molecular oxygen by N2O. In the present article, it will be shown that with promoted NiO catalysts, and using N2O, high activity, comparable with that of conventional O2-assisted ODH of ethane, is achieved. Furthermore, the use of the appropriate dopant, such as niobium, allows high ethylene yields (40 %), with a selectivity to ethylene of 72 % at 55 % ethane conversion. Overall, the catalytic results obtained indicate that the presence/absence and the nature of the promoter determines the catalytic performance of NiO based catalysts and the selectivity to ethylene can be explained on the basis of the electrochemical properties of the catalysts, correlating with parameters such as the density of acceptor defects (cationic vacancies) and the charge-transfer resistance at the interfacial active sites of the catalysts. Interestingly, the most selective catalyst (i.e., Nb-doped NiO) is highly robust as it presents stable catalytic performance after 24 h online and Ni2+ species are not reduced to Ni0 even working at high temperatures in N2O-free conditions.