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The coverage of H-MFI zeolite acid sites by light alkanes (C 3–C 7) at monomolecular cracking reaction conditions was determined using infrared operando spectroscopy. Under such conditions, alkane adsorption through H-bonding leads to a fully reversible perturbation of the zeolite νOH band at 3600 cm –1. This was used to assess the coverage at various temperatures and pressures, allowing for the determination of the adsorption thermodynamic parameters at reaction conditions.

Sep 28, 2004. Enzymes such as cytochrome P450, methane monooxygenase and alkane hydroxylase are able to catalyze the alkane oxidation to the corresponding alcohol. The range of alkanes recognized as substrates covers up to C24, depending on the enzymatic system used. The enzymatic alkane activation is. Interaction with hydrophobic substrates. Appl Environ Microbiol 66:3263–3268. Atlas RM (1981) Microbial degradation of petroleum hydrocarbons: an environmental. Microbiol Rev 45(1):180–209. Ayala M, Torres E (2004) Enzymatic activation of alkanes: constraints and prospective. Inasmuch as nearly all transition-state barriers are narrow near their summits, enzyme dynamics is an attractive way to lower the activation energy by altering the. We usually think of nucleophiles as a species with high-lying lowest occupied molecular orbitals (e. Wurlitzer Cornet Serial Numbers there. g., lone-pair orbitals or the p-orbitals in alkenes or aromatic. Suicide inactivation of peroxidases and the challenge of engineering more robust enzymes. B Valderrama, M Ayala, R Vazquez. Enzymatic activation of alkanes: constraints and prospective. M Ayala, E Torres. The prospects for peroxidase-based biorefining of petroleum fuels. M Ayala, J Verdin, R Vazquez-.

The simultaneous determination of apparent monomolecular cracking rate constants allowed for the direct determination of the intrinsic cracking rate constants, activation energies, and activation entropies. These results show that while the coverage of the active sites increases with the alkane size, the differences tend to decrease at high temperature because of entropic effects. The intrinsic activation energy was constant for all alkanes investigated in this study (∼190 kJ mol –1), lying in the lower range of the values usually derived from alkane adsorption heats and apparent activation energies.

The magnitude of the activation entropies obtained in the present study was also lower than those derived from low temperature adsorption measurements, indicating that temperature could increase the entropy of the adsorbed state. However, this decrease was much less dramatic than that predicted by recent state of art simulations. In any case, this operando study confirms that the activation entropy chiefly determines the variations of apparent protolytic cracking rates. Learn more about these metrics Article Views are the COUNTER-compliant sum of full text article downloads since November 2008 (both PDF and HTML) across all institutions and individuals.