Role of Catalyst Preparation on the Electrocatalytic Activity of Ni1–xFexOOH for the Oxygen Evolution Reaction

Klaus, Shannon; Louie, Mary W.; Trotochaud, Lena; Bell, Alexis T.

doi:10.1021/acs.jpcc.5b04776

Role of Catalyst Preparation on the Electrocatalytic Activity of Ni_1–xFe_xOOH for the Oxygen Evolution Reaction

Journal Article · Sun Jul 19 00:00:00 EDT 2015 · Journal of Physical Chemistry. C

DOI:https://doi.org/10.1021/acs.jpcc.5b04776· OSTI ID:1512218

Klaus, Shannon ^[1]; Louie, Mary W. ^[1]; Trotochaud, Lena ^[1]; Bell, Alexis T. ^[1]

Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Univ. of California, Berkeley, CA (United States)

Ni_1–xFe_xOOH thin films prepared via cathodic electrodeposition have been demonstrated to be highly active catalysts for the oxygen evolution reaction (OER) in basic media. Integration of these catalysts with light-absorbing semiconductors is required for photoelectrochemical fuel generation. However, the application of cathodic potentials required for typical electrochemical catalyst deposition limits the library of compatible photoanode materials. Sputter deposition of catalysts circumvents this limitation by enabling facile catalyst layering without cathodic potentials. In this work, we compare the structure and OER activity of sputter-deposited and electrodeposited Ni_1–xFe_xOOH thin films. Electrochemical cycling converts sputtered Ni_1-xFe_x metallic films to the desired oxides/(oxy)hydroxides. Both film preparation methods give catalysts with similar electrochemical behavior across all compositions. Additionally, OER activity is comparable between the deposition methods, with maximum activity for films with ~20% Fe content (320 mV overpotential at j = 10 mA cm^-2 geometric). Electrochemical cycling to convert sputtered metallic Ni_1-xFe_x films to metal oxides/(oxy)hydroxides is found to lower the Fe/Ni ratio, while the electrodeposited films exhibit comparable Fe/Ni ratios before and after electrochemical cycling and characterization. Structurally, Fe is found to incorporate within the Ni(OH)₂/NiOOH lattice for films formed through both sputter-deposition and electrodeposition. Layered films were also compared to codeposited 1:1 Fe/Ni films. It is found that, for layered films, an Fe top layer inhibits the electrochemical conversion of metallic Ni to Ni(OH)₂/NiOOH, thus reducing the amount of Ni_1–xFe_xOOH OER-active phase formed. In contrast, migration of metals within Ni-on-top films occurs readily during electrochemical cycling, resulting in films that are structurally and electrochemically indistinguishable from codeposited Ni_1–xFe_xOOH. These findings enable direct application of Ni_1–xFe_xOOH sputtered films to a wider library of photoanodes for light-driven water-splitting applications.

View Accepted Manuscript (DOE)

Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22), Chemical Sciences, Geosciences & Biosciences Division (SC-22.1)

Grant/Contract Number:: AC02-05CH11231

OSTI ID:: 1512218

Journal Information:: Journal of Physical Chemistry. C, Journal Name: Journal of Physical Chemistry. C Journal Issue: 32 Vol. 119; ISSN 1932-7447

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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