Structure sensitivity of n-butane hydrogenolysis on supported Ir catalysts

Zhang, Xiwen; Lu, Yubing; Kovarik, Libor; Dasari, Prasanna; Nagaki, Dick; Karim, Ayman M.

doi:10.1016/j.jcat.2020.10.028

Structure sensitivity of n-butane hydrogenolysis on supported Ir catalysts

Journal Article · Fri Nov 06 00:00:00 EST 2020 · Journal of Catalysis

DOI:https://doi.org/10.1016/j.jcat.2020.10.028· OSTI ID:1843225

^[1]; Lu, Yubing ^[1]; ^[2]; ^[3]; Nagaki, Dick ^[3]; ^[1]

Virginia Polytechnic Inst. and State Univ. (Virginia Tech), Blacksburg, VA (United States)
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
SABIC, Sugar Land, TX (United States)

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 ~1.4–1.6 nm and then drops with a further increase in particle size. In this work, the product distribution at low temperature (170–190 °C) is dominated by central and terminal CAC bond cleavage of n-butane, and less by two CAC bond cleavage or further hydrogenolysis of the propane and ethane products. The selectivity to central CAC bond cleavage is highly dependent on the size of Ir and increases with a decrease in particle size down to ~1.4 nm but remains constant with further decrease in size. The results show that an Ir size of ~1.4 nm is optimum for n-butane hydrogenolysis activity and selectivity towards ethane.

View Accepted Manuscript (DOE)

Research Organization:: Pacific Northwest National Laboratory (PNNL), Richland, WA (United States). Environmental Molecular Sciences Laboratory (EMSL)

Sponsoring Organization:: Sabic; USDOE

Grant/Contract Number:: AC05-76RL01830

OSTI ID:: 1843225

Report Number(s):: PNNL-SA-158239

Journal Information:: Journal of Catalysis, Journal Name: Journal of Catalysis Vol. 394; ISSN 0021-9517

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
alkane hydrogenolysis
heterogeneous catalyst
infrared spectroscopy
structure sensitivity
supported iridium nanoparticles

Structure sensitivity of n-butane hydrogenolysis on supported Ir catalysts

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