Capturing the Coverage Dependence of Aromatics' Adsorption through Mean-Field Models

Naseeha Cardwell; Alyssa J R Hensley; Yong Wang; Jean-Sabin McEwen

doi:10.1021/acs.jpca.3c05456

Capturing the Coverage Dependence of Aromatics' Adsorption through Mean-Field Models

J Phys Chem A. 2023 Dec 21;127(50):10693-10700. doi: 10.1021/acs.jpca.3c05456. Epub 2023 Dec 7.

Authors

Naseeha Cardwell¹, Alyssa J R Hensley^{1

2}, Yong Wang^{1

3}, Jean-Sabin McEwen^{1

3

4

5

6}

Affiliations

¹ The Gene and Linda Voiland School of Chemical Engineering and Bioengineering, Washington State University, Pullman, Washington 99164, United States.
² Department of Chemical Engineering & Materials Science, Stevens Institute of Technology, Hoboken, New Jersey 07030, United States.
³ Institute for Integrated Catalysis, Pacific Northwest National Laboratory, Richland, Washington 99352, United States.
⁴ Department of Physics and Astronomy, Washington State University, Pullman, Washington 99164, United States.
⁵ Department of Chemistry, Washington State University, Pullman, Washington 99164, United States.
⁶ Department of Biological Systems Engineering, Washington State University, Pullman, Washington 99164, United States.

PMID: 38059355
DOI: 10.1021/acs.jpca.3c05456

Abstract

To capture the dominant interactions (surface-mediated and through-space) in catalytic hydrodeoxygenation systems, coverage-dependent mean-field models of aromatic adsorption are developed on Pt(111) and Ru(0001). We derive three key insights from this work: (1) we can universally apply mean-field models to capture the coverage-dependent behavior of oxygenated aromatics on transition-metal surfaces, (2) we can deconvolute surface-mediated and through-space interactions from the mean-field model, and (3) we can develop relatively accurate models that predict the adsorption energy of aromatics on transition-metal surfaces for the full coverage range using the work function at the lowest modeled coverage. Our approach enables the rapid prediction of the coverage-dependent behavior of oxygenated aromatics on transition-metal surfaces, reducing the computational cost associated with these studies by an order of magnitude.