4.8 Article

Structure sensitivity of n-butane hydrogenolysis on supported Ir catalysts

Journal

JOURNAL OF CATALYSIS
Volume 394, Issue -, Pages 376-386

Publisher

ACADEMIC PRESS INC ELSEVIER SCIENCE
DOI: 10.1016/j.jcat.2020.10.028

Keywords

Alkane hydrogenolysis; Structure sensitivity; Heterogeneous catalyst; Supported iridium nanoparticles; Infrared spectroscopy

Funding

  1. Sabic
  2. U.S. Department of Energy, office of Biological and Environmental Research [49326]

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Hydrogenolysis of alkanes on transition metal heterogeneous catalysts is structure sensitive, with Ir particle size affecting n-butane hydrogenolysis activity. Results show that larger Ir particle sizes within the 1-3 nm range lead to increased activity, peaking around 1.4-1.6 nm before decreasing. At low temperatures, product distribution is dominated by central and terminal C-C bond cleavage, with selectivity depending on the size of Ir particles, increasing with sizes smaller than 1.4 nm.
Hydrogenolysis of alkanes has been widely reported as structure sensitive reaction on transition metal heterogeneous catalysts with metal particle sizes ranging between 1 and 20 nm. In this work, a series of Ir/MgAl2O4 and Ir/SiO2 catalysts with different Ir particle sizes ranging from subnanometer clusters (<1 nm) to nanoparticles (1-3 nm) were prepared and tested for n-butane hydrogenolysis. Our results show that the activity towards n-butane hydrogenolysis increases as Ir particle size increases in the lower particle size range, goes through a maximum at similar to 1.4-1.6 nm and then drops with a further increase in particle size. The product distribution at low temperature (170-190 degrees C) is dominated by central and terminal C-C bond cleavage of n-butane, and less by two C-C bond cleavage or further hydrogenolysis of the propane and ethane products. The selectivity to central C-C bond cleavage is highly dependent on the size of Ir and increases with a decrease in particle size down to similar to 1.4 nm but remains constant with further decrease in size. The results show that an Ir size of similar to 1.4 nm is optimum for n-butane hydrogenolysis activity and selectivity towards ethane. (C) 2020 Elsevier Inc. All rights reserved.

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