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Unraveling the Role of Particle Size and Nanostructuring on the Oxygen Evolution Activity of Fe-Doped NiO.
Rao, Reshma R; Bucci, Alberto; Corby, Sacha; Moss, Benjamin; Liang, Caiwu; Gopakumar, Aswin; Stephens, Ifan E L; Lloret-Fillol, Julio; Durrant, James R.
Afiliación
  • Rao RR; Department of Materials, Royal School of Mines, Imperial College London, South Kensington Campus, London SW7 2AZ, U.K.
  • Bucci A; Grantham Institute-Centre for Climate Change and the Environment, Imperial College London, South Kensington Campus, London SW7 2AZ, U.K.
  • Corby S; Institute of Chemical Research of Catalonia (ICIQ), The Barcelona Institute of Science and Technology, Avinguda Països Catalans 16, Tarragona 43007, Spain.
  • Moss B; Department of Chemistry, Centre for Processable Electronics, Imperial College London, London W12 0BZ, U.K.
  • Liang C; Department of Chemistry, Centre for Processable Electronics, Imperial College London, London W12 0BZ, U.K.
  • Gopakumar A; Department of Materials, Royal School of Mines, Imperial College London, South Kensington Campus, London SW7 2AZ, U.K.
  • Stephens IEL; Institute of Chemical Research of Catalonia (ICIQ), The Barcelona Institute of Science and Technology, Avinguda Països Catalans 16, Tarragona 43007, Spain.
  • Lloret-Fillol J; Department of Materials, Royal School of Mines, Imperial College London, South Kensington Campus, London SW7 2AZ, U.K.
  • Durrant JR; Institute of Chemical Research of Catalonia (ICIQ), The Barcelona Institute of Science and Technology, Avinguda Països Catalans 16, Tarragona 43007, Spain.
ACS Catal ; 14(15): 11389-11399, 2024 Aug 02.
Article en En | MEDLINE | ID: mdl-39114087
ABSTRACT
Nickel-based oxides and oxyhydroxide catalysts exhibit state-of-the-art activity for the sluggish oxygen evolution reaction (OER) under alkaline conditions. A widely employed strategy to increase the gravimetric activity of the catalyst is to increase the active surface area via nanostructuring or decrease the particle size. However, the fundamental understanding about how tuning these parameters influences the density of oxidized species and their reaction kinetics remains unclear. Here, we use solution combustion synthesis, a low-cost and scalable approach, to synthesize a series of Fe0.1Ni0.9O samples from different precursor salts. Based on the precursor salt, the nanoparticle size can be changed significantly from ∼2.5 to ∼37 nm. The OER activity at pH 13 trends inversely with the particle size. Using operando time-resolved optical spectroscopy, we quantify the density of oxidized species as a function of potential and demonstrate that the OER kinetics exhibits a second-order dependence on the density of these species, suggesting that the OER mechanism relies on O-O coupling between neighboring oxidized species. With the decreasing particle size, the density of species accumulated is found to increase, and their intrinsic reactivity for the OER is found to decrease, attributed to the stronger binding of *O species (i.e., a cathodic shift of species energetics). This signifies that the high apparent OER activity per geometric area of the smaller nanoparticles is driven by their ability to accumulate a larger density of oxidized species. This study not only experimentally disentangles the influence of the density of oxidized species and intrinsic kinetics on the overall rate of the OER but also highlights the importance of tuning these parameters independently to develop more active OER catalysts.
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Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Idioma: En Revista: ACS Catal Año: 2024 Tipo del documento: Article Pais de publicación: Estados Unidos
Texto completo
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Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Idioma: En Revista: ACS Catal Año: 2024 Tipo del documento: Article Pais de publicación: Estados Unidos