Engendering Unprecedented Activation of Oxygen Evolution via Rational Pinning of Ni Oxidation State in Prototypical Perovskite: Close Juxtaposition of Synthetic Approach and Theoretical Conception
Research output: Contribution to journal › Journal article › Research › peer-review
Documents
- Fulltext
Accepted author manuscript, 3.77 MB, PDF document
Rational optimization of the OER activity of catalysts based on LaNiO3 oxide is achieved by maximizing the presence of trivalent Ni in the surface structure. DFT investigations of the LaNiO3 catalyst and surface structures related to it predict an improvement in the OER activity for these materials to levels comparable with the top of the OER volcano if the La content is minimized while the oxidation state of Ni is maintained. These theoretically predicted structures of high intrinsic OER activity can be prepared by a templated sprayfreeze freeze-drying synthesis followed by a simple postsynthesis exfoliation-like treatment in acidic media. These nanocrystalline LaNiO3-related materials confirm the theoretical predictions, showing a dramatic improvement in OER activity. The exfoliated surfaces remain stable in OER catalysis, as shown by an in-operando ICP-OES study. The unprecedented OER activation of the synthesized LaNiO3 based materials is related to a close juxtaposition of the theoretical conception of ideal structural motifs and the ability to engender such motifs using a unique synthetic procedure, both principally related to stabilization and pinning of the Ni oxidation state within the local coordination environment of the perovskite structure.
Original language | English |
---|---|
Journal | ACS Catalysis |
Volume | 11 |
Issue number | 2 |
Pages (from-to) | 985-997 |
Number of pages | 13 |
ISSN | 2155-5435 |
DOIs | |
Publication status | Published - 15 Jan 2021 |
- electrocatalysis, oxygen evolution, rational catalyst design, DFT, ELECTROCATALYTIC ACTIVITY, RECENT PROGRESS, WATER, ALKALINE, LANIO3, CATALYSTS, NICKEL, NANOCRYSTALS, RUO2, NANOPARTICLES
Research areas
Number of downloads are based on statistics from Google Scholar and www.ku.dk
ID: 286635775