Direct Deoxygenation of Phenol over Fe-Based Bimetallic Surfaces Using On-the-Fly Surrogate Models

Onyango, Isaac; Zhu, Qiang

doi:10.1021/acs.jpcc.5c05436

Direct Deoxygenation of Phenol over Fe-Based Bimetallic Surfaces Using On-the-Fly Surrogate Models

Journal Article · Mon Oct 13 00:00:00 EDT 2025 · Journal of Physical Chemistry. C

DOI:https://doi.org/10.1021/acs.jpcc.5c05436· OSTI ID:3005777

^[1]; Zhu, Qiang ^[2]

North Carolina Battery Complexity, Autonomous Vehicle and Electrification (BATT CAVE) Research Center, Charlotte, NC (United States)
University of North Carolina at Charlotte, NC (United States)

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 result in significantly higher reverse reaction rates, making DDO unfavorable on these surfaces. This work demonstrates the effectiveness of GRR-accelerated transition state searches for complex surface reactions and provides insights into rational design of bimetallic catalysts for selective deoxygenation.

View Accepted Manuscript (DOE)

Research Organization:: Chicago Office, Argonne, IL (United States); University of North Carolina at Charlotte, NC (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0024866

OSTI ID:: 3005777

Alternate ID(s):: OSTI ID: 2997640
OSTI ID: 3000385

Journal Information:: Journal of Physical Chemistry. C, Journal Name: Journal of Physical Chemistry. C Journal Issue: 42 Vol. 129; ISSN 1932-7455; ISSN 1932-7447

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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