期刊
CHEMPHYSCHEM
卷 23, 期 7, 页码 -出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/cphc.202200072
关键词
heterogeneous catalysis; hydrogenation; hyperpolarization; methylenecyclobutane; NMR spectroscopy; parahydrogen
资金
- Russian Foundation for Basic Research [19-29-10003]
- RSF [21-73-10105]
- Russian Ministry of Science and Higher Education [AAAA-A16-116121510087-5]
- Russian Science Foundation [21-73-10105] Funding Source: Russian Science Foundation
In this study, the mechanism of methylenecyclobutane hydrogenation over titania-supported Rh, Pt, and Pd catalysts was investigated using parahydrogen-induced polarization (PHIP) technique. It was found that the reaction leads to the formation of a mixture of cyclic, linear, and branched compounds, and the temperature has a significant influence on the product composition.
In this work the mechanism of methylenecyclobutane hydrogenation over titania-supported Rh, Pt and Pd catalysts was investigated using parahydrogen-induced polarization (PHIP) technique. It was found that methylenecyclobutane hydrogenation leads to formation of a mixture of reaction products including cyclic (1-methylcyclobutene, methylcyclobutane), linear (1-pentene, cis-2-pentene, trans-2-pentene, pentane) and branched (isoprene, 2-methyl-1-butene, 2-methyl-2-butene, isopentane) compounds. Generally, at lower temperatures (150-350 degrees C) the major reaction product was methylcyclobutane while higher temperature of 450 degrees C favors the formation of branched products isoprene, 2-methyl-1-butene and 2-methyl-2-butene. PHIP effects were detected for all reaction products except methylenecyclobutane isomers 1-methylcyclobutene and isoprene implying that the corresponding compounds can incorporate two atoms from the same parahydrogen molecule in a pairwise manner in the course of the reaction in particular positions. The mechanisms were proposed for the formation of these products based on PHIP results.
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