Selective Acetylene Hydrogenation over Single-Atom Alloy Nanoparticles by Kinetic Monte Carlo
Journal article, 2019

Single-atom alloys, which are prepared byembedding isolated metal sites in host metals, are promisingsystems for improved catalyst selectivity. For technical applications, catalysts based on nanoparticles are preferred thanks to a large surface area. Herein, we investigate hydrogenation of acetylene to ethylene using kinetic MonteCarlo simulations based on density functional theory and compare the performance of Pd/Cu nanoparticles with Pd(111) and Pd/Cu(111). We find that embedding Pd in Cu systems strongly enhances the selectivity and that the reaction mechanism is fundamentally different for nanoparticles and extended surfaces. The reaction mechanism on nanoparticles is complex and involves elementary steps that proceed preferentially over different sites. Edge and corner sites on nanoparticles are predicted to lower the selectivity, and we infer that a rational design strategy in selective acetylene hydrogenation is to maximize the number of (111) sites in relation to edge sites for Pd/Cu nanoparticles.


Mikkel Jørgensen

Competence Centre for Catalysis (KCK)

Chalmers, Physics, Chemical Physics

Henrik Grönbeck

Chalmers, Physics, Chemical Physics

Competence Centre for Catalysis (KCK)

Journal of the American Chemical Society

0002-7863 (ISSN) 1520-5126 (eISSN)

Vol. 141 21 8541-8549

Catalytic activity from first principles

Swedish Research Council (VR) (2016-05234), 2017-01-01 -- 2020-12-31.

Subject Categories

Polymer Chemistry

Biochemistry and Molecular Biology

Atom and Molecular Physics and Optics

Areas of Advance

Nanoscience and Nanotechnology (SO 2010-2017, EI 2018-)


C3SE (Chalmers Centre for Computational Science and Engineering)





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