Journal
CHEMSUSCHEM
Volume 14, Issue 6, Pages 1595-1601Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/cssc.202002782
Keywords
mixed metal oxides; spinels; oxygen vacancy; water splitting; descriptors
Funding
- European Union under the H2020 FET-PROACT A-LEAF project [732840]
- Barcelona Supercomputing Center [QCM-2018-3-0012]
- Generalitat de Catalunya [2017 SGR 327]
- Spanish MINECO coordinated project VALPEC [ENE2017-85087-C3]
- Severo Ochoa program from Spanish MINECO [SEV-2017-0706]
- CERCA Programme / Generalitat de Catalunya
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The study investigates Fe-Ni-Zn spinel oxides as a platform for understanding the key contributions to oxygen evolution reaction (OER) electrocatalysis, finding that the presence of Zn in the spinel structure and the density of specific equimolar stoichiometric sites play crucial roles in maximizing OER performance. The work demonstrates cooperative electronic effects on surface active sites as essential for designing optimal OER electrocatalysts.
Sustainable electrocatalysis of the oxygen evolution reaction (OER) constitutes a major challenge for the realization of green fuels. Oxides based on Ni and Fe in alkaline media have been proposed to avoid using critical raw materials. However, their ill-defined structures under OER conditions make the identification of key descriptors difficult. Here, we have studied Fe-Ni-Zn spinel oxides, with a well-defined crystal structure, as a platform to obtain general understanding on the key contributions. The OER reaches maximum performance when: (i) Zn is present in the Spinel structure, (ii) very dense, equimolar 1 : 1 : 1 stoichiometry sites appear on the surface as they allow the formation of oxygen vacancies where Zn favors pushing the electronic density that is pulled by the octahedral Fe and tetrahedral Ni redox pair lowering the overpotential. Our work proves cooperative electronic effects on surface active sites as key to design optimum OER electrocatalysts.
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