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Quantum chemical evidence is produced to show that dimerization of linear butenes and pentenes at zeolitic Brønsted sites in H‐MFI yields alkanes featuring cyclohexane rings rather than branched alkenes. The absence of any C=C double bond in the formed cyclic alkane explains the observations that oligomerization stops at the dimer. The calculated reaction enthalpies for the dimerization of 2‐pentene...
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