Lattice Oxygen Exchange Pathways in Nickel–Iron Metal–Organic Framework-Based Oxygen Evolution Electrocatalysts
Source abstract
Abstract
The oxygen evolution reaction (OER) is crucial for electrofuel production. Metal–hydroxide organic frameworks (MHOFs), a subset of metal–organic frameworks with oxyhydroxide-like layers interconnected via organic linkers, have shown great promise as OER electrocatalysts. This study investigates lattice oxygen exchange in four Ni- and Fe-substituted MHOFs with varying linker stabilities using 18 O isotope labeling combined with operando Raman spectroscopy. A negative correlation between 18 O/ 16 O lattice oxygen exchange and the OER activity is shown, with Fe ions further suppressing exchange. Operando X-ray spectroscopy (XAS) and UV–vis further reveals that lattice oxygen exchange primarily proceeds on reduced Ni 2+ sites, with higher linker stability preserving more Ni 2+ sites and promoting greater lattice oxygen exchange. Supported by density functional theory, the MHOF surface transforms into an OER-active MO x H y -like phase, explaining the negative correlation of lattice exchange with the OER activity. This work also identifies a noninnocent role of the Raman laser in inducing lattice oxygen exchange and offers critical insights into various lattice oxygen exchange pathways in MHOFs, demonstrating their distinction from the catalytic lattice oxygen evolution reaction mechanism.
Source: openalex_inverted_index · Quality: baseline
Research context
OpenAlex topics: Electrocatalysts for Energy Conversion · Metal-Organic Frameworks: Synthesis and Applications · Advanced Photocatalysis Techniques
SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.
Affiliations
Department of Materials Science and Engineering
Massachusetts Institute of Technology
Department of Chemical Engineering
Department Interface Design
Helmholtz-Zentrum Berlin für Materialien und Energie GmbH (HZB)
Energy Materials In Situ Laboratory Berlin (EMIL)
HZB
Department of Chemistry-Ångström Laboratory, Uppsala University, P.O. Box 538, SE-75121 Uppsala, Sweden
Diamond Light Source
Harwell Science and Innovation Campus
Department of Materials Science and Engineering, Solid State Physics, Ångström Laboratory, Uppsala University, P.O. Box 35, SE-75103 Uppsala, Sweden
Helmholtz Institute Erlangen-Nürnberg for Renewable Energy (HIERN)
Department of Chemistry and Pharmacy
Friedrich-Alexander-Universität Erlangen-Nürnberg (FAU)
Department of Chemistry
Department of Mechanical Engineering
Research Laboratory of Electronics
Funding
Basic Energy Sciences · Kungl. Ingenjörsvetenskapsakademien · Sweden-America Foundation · Stiftelsen Åforsk · Toyota Research Institute · Stiftelsen Blanceflor Boncompagni Ludovisi, född Bildt
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