کد مقاله کد نشریه سال انتشار مقاله انگلیسی نسخه تمام متن
61315 47575 2013 8 صفحه PDF دانلود رایگان
عنوان انگلیسی مقاله ISI
Isotopic transient analysis of the ethanol coupling reaction over magnesia
موضوعات مرتبط
مهندسی و علوم پایه مهندسی شیمی کاتالیزور
پیش نمایش صفحه اول مقاله
Isotopic transient analysis of the ethanol coupling reaction over magnesia
چکیده انگلیسی

Isotopic transient analysis of ethanol coupling to butanol over MgO in a fixed-bed reactor at 673 K revealed a surface coverage of adsorbed ethanol equivalent to about 50% of the exposed MgO atomic pairs. DRIFTS of ethanol reaction at 673 K confirmed that the surface was populated primarily with adsorbed ethoxide and hydroxide, presumably from the dissociative adsorption of ethanol. The coverage of reactive intermediates leading to butanol was an order of magnitude lower than that of adsorbed ethanol, and about half the surface base sites counted by adsorption of CO2. The intrinsic turnover frequency for the coupling reaction at 673 K determined by isotopic transient analysis was 0.04 s−1, which is independent of any assumptions about the nature of the active sites. Although the ethanol coupling reaction appears to involve aldol condensation of an aldehyde intermediate, the high coverage of ethanol under steady-state conditions apparently inhibits unproductive CC coupling reactions that deactivate the catalyst at high temperature.

Isotopic transient analysis of the ethanol coupling reaction to butanol on MgO at 673 K revealed that half of the surface is covered with adsorbed ethanol, identified as ethoxide by DRIFTS, whereas the surface coverage of reactive intermediates leading to butanol was an order of magnitude lower than that of ethoxide. The high coverage of ethoxide and hydroxide inhibited CC coupling reactions, such as aldol addition reactions, that occur readily on MgO and lead to deactivation.Figure optionsDownload high-quality image (65 K)Download as PowerPoint slideHighlights
► Acetaldehyde, butanol, and ethene were produced from ethanol on MgO at 673 K.
► Ethanol dissociatively adsorbed on MgO forming surface ethoxide and hydroxide species.
► The coverage of adsorbed ethanol was about 50% of surface MgO pairs.
► The coverage of coupling intermediates was an order of magnitude lower than ethanol.
► High coverage of ethoxide and hydroxide inhibited coupling reactions.

ناشر
Database: Elsevier - ScienceDirect (ساینس دایرکت)
Journal: Journal of Catalysis - Volume 298, February 2013, Pages 130–137
نویسندگان
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