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<p>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, <i>exo</i>-tetrahydrodicyclopentadiene (C<sub>10</sub>H<sub>16</sub>), undergoes catalytic decomposition on TiAlB NPs in a chemical microreactor to produce 1,3-cyclopentadiene (c-C<sub>5</sub>H<sub>6</sub>), cyclopentene (c-C<sub>5</sub>H<sub>8</sub>), and molecular hydrogen (H<sub>2</sub>) 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.</p>

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

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2025年7月23日

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  • 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

摘要

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.