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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Nature Portfolio
2025-07-01
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| Series: | Nature Communications |
| Online Access: | https://doi.org/10.1038/s41467-025-62112-2 |
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| author | 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 |
| author_facet | 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 |
| author_sort | Souvick Biswas |
| collection | DOAJ |
| description | 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. |
| format | Article |
| id | doaj-art-05c7adcb679b44a89508bf7cc4d4298f |
| institution | DOAJ |
| issn | 2041-1723 |
| language | English |
| publishDate | 2025-07-01 |
| publisher | Nature Portfolio |
| record_format | Article |
| series | Nature Communications |
| spelling | doaj-art-05c7adcb679b44a89508bf7cc4d4298f2025-08-20T03:05:06ZengNature PortfolioNature Communications2041-17232025-07-0116111310.1038/s41467-025-62112-2Unconventional low temperature decomposition of a saturated hydrocarbon over atomically-dispersed titanium-aluminum-boron catalystSouvick Biswas0Jack Cokas1Winston Gee2Dababrata Paul3Nureshan Dias4Harry W. T. Morgan5Matthew T. Finn6Bethany M. Hudak7Perrin M. Godbold8Christopher A. Klug9Albert Epshteyn10Anastassia N. Alexandrova11Musahid Ahmed12Ralf I. Kaiser13Department of Chemistry, University of Hawaii at ManoaDepartment of Chemistry and Biochemistry, University of California, Los AngelesDepartment of Chemistry and Biochemistry, University of California, Los AngelesDepartment of Chemistry, University of Hawaii at ManoaChemical Sciences Division, Lawrence Berkeley National LaboratoryDepartment of Chemistry and Biochemistry, University of California, Los AngelesChemistry Division, U.S. Naval Research LaboratoryMaterials Science and Technology Division, U.S. Naval Research LaboratoryNRC Postdoctoral Associate, Chemistry Division, U.S. Naval Research LaboratoryChemistry Division, U.S. Naval Research LaboratoryChemistry Division, U.S. Naval Research LaboratoryDepartment of Chemistry and Biochemistry, University of California, Los AngelesChemical Sciences Division, Lawrence Berkeley National LaboratoryDepartment of Chemistry, University of Hawaii at ManoaAbstract 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.https://doi.org/10.1038/s41467-025-62112-2 |
| spellingShingle | 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 Unconventional low temperature decomposition of a saturated hydrocarbon over atomically-dispersed titanium-aluminum-boron catalyst Nature Communications |
| title | Unconventional low temperature decomposition of a saturated hydrocarbon over atomically-dispersed titanium-aluminum-boron catalyst |
| title_full | Unconventional low temperature decomposition of a saturated hydrocarbon over atomically-dispersed titanium-aluminum-boron catalyst |
| title_fullStr | Unconventional low temperature decomposition of a saturated hydrocarbon over atomically-dispersed titanium-aluminum-boron catalyst |
| title_full_unstemmed | Unconventional low temperature decomposition of a saturated hydrocarbon over atomically-dispersed titanium-aluminum-boron catalyst |
| title_short | Unconventional low temperature decomposition of a saturated hydrocarbon over atomically-dispersed titanium-aluminum-boron catalyst |
| title_sort | unconventional low temperature decomposition of a saturated hydrocarbon over atomically dispersed titanium aluminum boron catalyst |
| url | https://doi.org/10.1038/s41467-025-62112-2 |
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