A Fundamental Relationship between Reaction Mechanism and Stability in Metal Oxide Catalysts for Oxygen Evolution
Citations Over TimeTop 10% of 2016 papers
Abstract
Rational design of efficient, stable oxygen evolution reaction (OER) catalysts is necessary for widespread adoption of electrochemical energy storage technologies. Achieving this goal requires elucidation of fundamental relationships between surface structure and reaction mechanism. Here we address this issue using ab initio computations to determine the surface structure and OER mechanism for LaNiO3, a perovksite oxide that exhibits high activity but low stability. We find a new OER mechanism in which lattice oxygen participation via reversible formation of surface oxygen vacancies is critical. We show that this mechanism has a lower reaction barrier compared to the generally proposed mechanism, leading to improved agreement with experimental data. Extending the study to La1–xSrxBO3 (B = transition metal), we demonstrate a transition to the lattice oxygen-mediated mechanism with decreasing catalyst stability. Our results suggest new approaches for next-generation catalysts design.
Related Papers
- → Rational Design of Rhodium–Iridium Alloy Nanoparticles as Highly Active Catalysts for Acidic Oxygen Evolution(2019)219 cited
- → Water Splitting: Rational Design and Construction of Cocatalysts for Semiconductor‐Based Photo‐Electrochemical Oxygen Evolution: A Comprehensive Review (Adv. Sci. 2/2019)(2019)11 cited
- Theoretical study on the alcoholization mechanism of benzothiadiazole(2005)
- Quantum Chemistry Study on the Reaction Mechanism of CH_2O and H(2005)
- The Study of the Reaction Mechanism for the CH_3+O_3 Reaction(2002)