Scaling of Transition State Vibrational Frequencies and Application of d-Band Theory to the Brønsted–Evans–Polanyi Relationship on Surfaces

Lansford, Joshua L.; Kurdziel, Sophia J.; Vlachos, Dionisios G.

doi:10.1021/acs.jpcc.0c09686

Scaling of Transition State Vibrational Frequencies and Application of d-Band Theory to the Brønsted–Evans–Polanyi Relationship on Surfaces

Journal Article · Mon Feb 08 00:00:00 EST 2021 · Journal of Physical Chemistry. C

DOI:https://doi.org/10.1021/acs.jpcc.0c09686· OSTI ID:2212400

Lansford, Joshua L. ^[1]; Kurdziel, Sophia J. ^[2]; ^[2]

University of Delaware, Newark, DE (United States); University of Delaware
University of Delaware, Newark, DE (United States)

Semiempirical energy relations provide a means of estimating thermodynamic properties. Specifically, linear scaling relationships (LSRs) and Brønsted–Evans–Polanyi (BEP) relationships correlate adsorption energies between adsorbates across surfaces and reaction energies with activation barriers, respectively. Although vibrational scaling relations (VSRs) exist between adsorbates at identical sites, scaling between vibrational frequencies of adsorbed local minima and transition states is lacking. Here, we present density functional theory calculations for AH_X (A = C, N, O) diffusions on transition metal surfaces and reveal linear scaling between frequencies of local minima and the transition state between those minima. Using d-band theory and linear muffin tin orbital theory (LMTO), we derive the slopes of these transition state vibrational scaling relations (TSVSRs) and, in so doing, provide a rigorous theory extending the original BEP relations developed for solution chemistry to surface chemistry. Furthermore, with a single reference DFT calculation, we predict the slopes and quantify uncertainty in the predictions.

View Accepted Manuscript (DOE)

Research Organization:: RAPID Manufacturing Institute, New York, NY (United States)

Sponsoring Organization:: National Science Foundation (NSF); USDOE Office of Energy Efficiency and Renewable Energy (EERE), Energy Efficiency Office. Advanced Materials & Manufacturing Technologies Office (AMMTO)

Grant/Contract Number:: EE0007888

OSTI ID:: 2212400

Alternate ID(s):: OSTI ID: 1848637

Journal Information:: Journal of Physical Chemistry. C, Journal Name: Journal of Physical Chemistry. C Journal Issue: 13 Vol. 125; ISSN 1932-7447

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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