How should we approach the study of different non-concerted lattice oxygen mechanisms (LOMs) for oxygen evolution reactions (OER) via density functional theory approach, and why is the pKa value significant in this context? For reference, please see the following paper: "Activating lattice oxygen redox reactions in metal oxides to catalyse oxygen evolution," Nature Chemistry, 9, 457–465 (2017). https://doi.org/10.1038/nchem.2695.
Chaitanya Kumar
Thank you very much for the detailed answer.I have a followup question:
I am conducting DFT-based VASP calculations to study the non-concerted lattice oxygen mechanism (NLOM) for the oxygen evolution reaction (OER). In the concerted lattice oxygen mechanism (CLOM), each reaction step involves coupled proton-electron transfer (CPET), typically referenced to the standard hydrogen electrode (SHE). However, in the non-concerted lattice oxygen mechanism, the proton and electron transfer steps are decoupled. This decoupling introduces a dependency of the proton transfer step on the pH of the system.
Can you guide me on how to theoretically calculate the Gibbs free energy of these decoupled proton and electron transfer steps? Specifically, I am looking for an approach to handle the decoupling of proton and electron transfer and account for the pH influence on the proton transfer step.
Best,
Beenish Ajmal.
Chaitanya Kumar
Thank you for your help! I need clarification regarding VASP calculations for systems involving proton and electron transfer LOM. Specifically:I have attached a scheme showing the concerted vs. non-concerted pathways as a reference for context.
Could you guide me on the appropriate approach for handling charges and solvation in these calculations?
I truly appreciate your guidance.
Best,
Beenish Bashir.
Chaitanya Kumar
Thank you very much for detailed explanation. It will be incredibly helpful in building the OER model via LOM.Best,
Beenish Ajmal.
Chaitanya Kumar
Can you please share any literature that discusses non-concerted mechanisms studied via DFT (as you discussed above)? I can assume some aspects, but having relevant literature would help me develop a more accurate model to calculate the charged intermediates during the reaction. Thank you very much for your assistance.Best,
Beenish Ajmal.
Chaitanya Kumar
Thank you for sharing the literature. It will be very helpful in building my model on decoupled electron transfer (ET) and proton transfer (PT) in OER. I truly appreciate your assistance once again.Best,
Beenish Ajmal.
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