Unconventional low temperature decomposition of a saturated hydrocarbon over atomically-dispersed titanium-aluminum-boron catalyst

Abstract Sonochemically-synthesized atomically-dispersed titanium-aluminum-boron nanopowder (TiAlB NP) exhibits a remarkable low-temperature catalytic activation of aliphatic C-H bonds at 750 K followed by C-C bond activation thus emerging as a potent low-cost alternative to expensive platinum group...

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Main Authors: Souvick Biswas, Jack Cokas, Winston Gee, Dababrata Paul, Nureshan Dias, Harry W. T. Morgan, Matthew T. Finn, Bethany M. Hudak, Perrin M. Godbold, Christopher A. Klug, Albert Epshteyn, Anastassia N. Alexandrova, Musahid Ahmed, Ralf I. Kaiser
Format: Article
Language:English
Published: Nature Portfolio 2025-07-01
Series:Nature Communications
Online Access:https://doi.org/10.1038/s41467-025-62112-2
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Summary:Abstract Sonochemically-synthesized atomically-dispersed titanium-aluminum-boron nanopowder (TiAlB NP) exhibits a remarkable low-temperature catalytic activation of aliphatic C-H bonds at 750 K followed by C-C bond activation thus emerging as a potent low-cost alternative to expensive platinum group metals. Here, the model saturated hydrocarbon, exo-tetrahydrodicyclopentadiene (C10H16), undergoes catalytic decomposition on TiAlB NPs in a chemical microreactor to produce 1,3-cyclopentadiene (c-C5H6), cyclopentene (c-C5H8), and molecular hydrogen (H2) as detected in situ via isomer-selective, single-photon ionization time-of-flight mass spectrometry. Extensive electronic structure theory calculations on model clusters of the catalyst decode a unique synergy among the atomic constituents of the catalyst and chemical bonding in this stepwise, retro Diels Alder reaction: Ti, although insensitive to C-H activation in its metallic state, initiates the catalysis via chemisorption of the hydrocarbon, adjacent B centers readily abstract hydrogen atoms and store them during the catalytic cycle, while Al stabilizes the catalyst structure yet providing space for critical docking sites for the departing hydrocarbons.
ISSN:2041-1723