Difference in the Catalytic Activity of Atoms in the Corners and at the Edges of Gold Nanoparticles: Hydrogen Isotope Exchange Reaction

金纳米粒子角部和边缘原子催化活性的差异:氢同位素交换反应

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Abstract

The goal of this work is to investigate the catalytic activities of low-coordination atoms located in gold nanoparticles. Gold nanoparticles with sizes from 0.7 to 40 nm deposited on γ-Al(2)O(3) were used as a catalyst. Synthesized gold nanoparticles and prepared catalysts were characterized by HRTEM, SEM, XRD, DLS, and UV-Vis spectroscopy. The specific activity of gold nanoparticles towards the isotope exchange reaction at 77 K was studied as a function of nanoparticle size. The catalytic activity increases significantly when the particle size is less than 3 nm. The activities of low-coordination gold atoms located at the edges and in the corners are markedly different. Corner atoms (CN = 6) are more than 40 times more active in the reaction of hydrogen isotope exchange than edge atoms (CN = 7). TOF for atoms with coordination numbers CN = 6 and CN = 7 are 0.258 ± 0.020 and 0.006 ± 0.001 molecules site(-1) s(-1), respectively. An equation was proposed for the dependence of the catalytic activity of the reaction on the particle size, the number of atoms on the surface, and their activity.

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