Altering Linear Scaling Relationships on Metal Catalysts via Ligand–Adsorbate Hydrogen Bonding

Jenkins, Alexander H.; Musgrave, Charles B.; Medlin, J. Will

doi:10.1021/acs.jpcc.1c07550

Title: Altering Linear Scaling Relationships on Metal Catalysts via Ligand–Adsorbate Hydrogen Bonding

Journal Article · 21 October 2021 · Journal of Physical Chemistry. C

DOI: https://doi.org/10.1021/acs.jpcc.1c07550 · OSTI ID:1866622

Jenkins, Alexander H. ^[1];

^[2];

^[2]

Univ. of Colorado, Boulder, CO (United States); University of Colorado Boulder
Univ. of Colorado, Boulder, CO (United States)

Linear scaling relationships for adsorption energies of related molecules provide a simple tool for the prediction of catalytic properties and also reveal inherent constraints in heterogeneous catalyst design. In an effort to predict materials that preferentially stabilize intermediates capable of forming hydrogen bonds (H-bonds) and thus reduce these constraints, scaling relations for thiolate-coated fcc (111) surfaces were developed. Here, we demonstrate how ligand–adsorbate H-bonds lead to the stabilization of certain adsorbates and how this affects the linear scaling of adsorption energies for similarly bound intermediates. For H-bonds that occur remote from the surface, ligand–adsorbate H-bond strength is independent of metal composition and instead depends only on the acidities of the H-bond-forming functional groups. As the distance of H-bond-accepting groups from the surface decreases and interactions with the metal strengthen, the effect of surface composition on H-bond strength increases while additional factors, such as conformational changes and steric hinderance, can offset the stabilizing effect of the ligands. In this work, these competing factors may influence both the slope and y-intercept of adsorption strength scaling. These findings aid the rational design of enhanced catalytic materials by enabling the screening of ligand- or spectator-modified materials that do not conform to the linear scaling relations of bare metal surfaces.

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Research Organization:: Univ. of Colorado, Boulder, CO (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF)

Grant/Contract Number:: SC0005239

OSTI ID:: 1866622

Journal Information:: Journal of Physical Chemistry. C, Journal Name: Journal of Physical Chemistry. C Journal Issue: 43 Vol. 125; ISSN 1932-7447

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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