Direct Deoxygenation of Phenol over Fe-Based Bimetallic Surfaces Using On-the-Fly Surrogate Models
Isaac Onyango, Qiang Zhu
TL;DR
This paper uses a fast computational method to study how phenol loses oxygen on iron-based surfaces, showing how adding metals like cobalt and nickel affects the reaction.
Contribution
The study introduces a Gaussian process regression calculator that accelerates transition state searches with high accuracy for surface reactions.
Findings
Subsurface Co and Ni substitutions maintain favorable DDO thermodynamics and kinetics similar to pure Fe(110).
Top-layer Co and Ni substitutions increase C–O bond cleavage barriers and make DDO unfavorable.
GPR-NEB provides up to 3 times speedup over DFT with energy barrier errors below 0.015 eV.
Abstract
We present an accelerated nudged elastic band (NEB) study of phenol direct deoxygenation (DDO) on Fe-based bimetallic surfaces using a recently developed Gaussian process regression (GPR) calculator. Our test calculations demonstrate that the GPR calculator achieves up to 3 times speedup compared to conventional density functional theory calculations while maintaining high accuracy, with energy barrier errors below 0.015 eV. Using GPR-NEB, we systematically examine the DDO mechanism on pure Fe(110) and surfaces modified with Co and Ni in both top and subsurface layers. Our results show that subsurface Co and Ni substitutions preserve favorable thermodynamics and kinetics for both C–O bond cleavage and C–H bond formation, comparable to those on the pure Fe(110) surface. In contrast, top-layer substitutions generally increase the C–O bond cleavage barrier, render the step endothermic, and…
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Taxonomy
TopicsCatalytic Processes in Materials Science · Catalysis and Oxidation Reactions · Environmental remediation with nanomaterials