Influence of adsorbates on the electronic structure, bond strain, and thermal properties of an alumina-supported Pt catalyst

ACS Nano
Matthew W SmallRalph G Nuzzo

Abstract

We describe the results of an X-ray absorption spectroscopy (XAS) study of adsorbate and temperature-dependent alterations of the atomic level structure of a prototypical, noble metal hydrogenation and reforming catalyst: ∼1.0 nm Pt clusters supported on gamma alumina (Pt/γ-Al(2)O(3)). This work demonstrates that the metal-metal (M-M) bonding in these small clusters is responsive to the presence of adsorbates, exhibiting pronounced coverage-dependent strains in the clusters' M-M bonding, with concomitant modifications of their electronic structures. Hydrogen and CO adsorbates demonstrate coverage-dependent bonding that leads to relaxation of the M-M bond strains within the clusters. These influences are partially compensated, and variably mediated, by the temperature-dependent electronic perturbations that arise from cluster-support and adsorbate-support interactions. Taken together, the data reveal a strikingly fluxional system with implications for understanding the energetics of catalysis. We estimate that a 9.1 ± 1.1 kJ/mol strain exists for these clusters under H(2) and that this strain increases to 12.8 ± 1.7 kJ/mol under CO. This change in the energy of the particle is in addition to the different heats of adsorption for...Continue Reading

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Citations

Jun 14, 2013·The Journal of Chemical Physics·Zhanghui ChenShushen Li
Mar 14, 2013·Journal of Computational Chemistry·Zhanghui ChenLinwang Wang
Mar 19, 2014·Chemphyschem : a European Journal of Chemical Physics and Physical Chemistry·Matthew W SmallAnatoly I Frenkel
Jan 2, 2016·The Journal of Physical Chemistry Letters·Lin LiJens K Nørskov
Jul 23, 2013·Journal of the American Chemical Society·Long LiJudith C Yang
Oct 26, 2016·Langmuir : the ACS Journal of Surfaces and Colloids·Olga A Yakovina, Alexander S Lisitsyn
Sep 23, 2014·Physical Review Letters·Thomas N JensenJeppe V Lauritsen
Sep 29, 2020·Chemical Reviews·Janis Timoshenko, Beatriz Roldan Cuenya
Oct 5, 2021·Physical Chemistry Chemical Physics : PCCP·Alexander S Lisitsyn, Anastasiya S Kadtsyna
Oct 30, 2021·ACS Applied Materials & Interfaces·Haodong WangAnatoly I Frenkel

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