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Ternary Ni-Co-Fe oxyhydroxide oxygen evolution catalysts: Intrinsic activity trends, electrical conductivity, and electronic band structure

Stevens, Michaela Burke ; Enman, Lisa J. ; Korkus, Ester Hamal ; Zaffran, Jeremie ; Trang, Christina D. M. ; Asbury, James ; Kast, Matthew G. ; Toroker, Maytal Caspary ; Boettcher, Shannon W.

Nano research, 2019-09, Vol.12 (9), p.2288-2295 [Revista revisada por pares]

Beijing: Tsinghua University Press

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Título:
Ternary Ni-Co-Fe oxyhydroxide oxygen evolution catalysts: Intrinsic activity trends, electrical conductivity, and electronic band structure
Autor: Stevens, Michaela Burke ; Enman, Lisa J. ; Korkus, Ester Hamal ; Zaffran, Jeremie ; Trang, Christina D. M. ; Asbury, James ; Kast, Matthew G. ; Toroker, Maytal Caspary ; Boettcher, Shannon W.
Materias: Atomic/Molecular Structure and Spectra ; Biomedicine ; Biotechnology ; Catalysis ; Catalysts ; Chemical elements ; Chemistry and Materials Science ; Cobalt ; Composition ; Condensed Matter Physics ; Conductivity ; Electrical conductivity ; Electrical resistivity ; Electrocatalysts ; Electrolytes ; Electronic structure ; Emission measurements ; Emission spectroscopy ; Heavy metals ; Hybridization ; Hydroxides ; Inductively coupled plasma ; Iron ; Materials Science ; Mathematical analysis ; Metals ; Nanotechnology ; Nickel ; Optical emission spectroscopy ; Organic chemistry ; Oxygen ; Oxygen evolution reactions ; Research Article ; Spectroscopy ; Structure-activity relationships ; Synergism ; Valence band
Es parte de: Nano research, 2019-09, Vol.12 (9), p.2288-2295
Descripción: Nickel-, cobalt-, and iron-based (oxy)hydroxides comprise the most-commonly studied electrocatalysts for the oxygen-evolution reaction (OER) in alkaline solution. A fundamental understanding of composition-structure-activity relationships for mixed-metal Ni-Co and Ni-Co-Fe (oxy)hydroxides is important to guide the design of advanced OER catalysts. Here we use cyclic voltammetry, chronopotentiometry, inductively-coupled plasma-optical emission spectroscopy, and in situ electrical conductivity measurements to characterize the properties and activity of various compositions of Ni-Co-Fe (oxy)hydroxides prepared by cathodic co-electrodeposition. Consistent with previous studies, we find Fe is essential for the mixed-metal (oxy)hydroxides to achieve high OER activity. In the rigorous absence of Fe (achieved by using specially cleaned electrolytes), the most-active Ni-Co (oxy)hydroxide composition has an OER turn-over frequency only twice that of pure Co (oxy)hydroxide, suggesting minimal synergism between the two metals. The addition of Co to Ni-Fe (oxy)hydroxides shifts the onset of electrical conductivity to lower potentials, but has little effect on the intrinsic OER activity, with the most-active Ni-Co-Fe (oxy)hydroxide having an OER turn-over frequency only ~ 1.5 times that of the Ni-Fe (oxy)hydroxides. The magnitudes of the electrical conductivities are similar for all the compositions measured. Density-functional-theory-calculated projected density of states show a significant contribution of all chemical elements at the valence band edge of the mixed-metal oxyhydroxide electronic structure, demonstrating significant electronic hybridization between the elements. The calculations suggest the involvement of all the elements in modulating the electronic structure at putative Fe-based active sites that are probably located at edges or defects in the two-dimensional oxyhydroxide sheets.
Editor: Beijing: Tsinghua University Press
Idioma: Inglés

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Ternary Ni-Co-Fe oxyhydroxide oxygen evolution catalysts: Intrinsic activity trends, electrical conductivity, and electronic band structure

Stevens, Michaela Burke ; Enman, Lisa J. ; Korkus, Ester Hamal ; Zaffran, Jeremie ; Trang, Christina D. M. ; Asbury, James ; Kast, Matthew G. ; Toroker, Maytal Caspary ; Boettcher, Shannon W.

Beijing: Tsinghua University Press

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