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A Combined Kinetic and Thermodynamic Approach for the Interpretation of Continuous‐Flow Heterogeneous Catalytic Processes
Author(s) -
Bortolini Olga,
Cavazzini Alberto,
Giovannini Pier Paolo,
Greco Roberto,
Marchetti Nicola,
Massi Alessandro,
Pasti Luisa
Publication year - 2013
Publication title -
chemistry – a european journal
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 1.687
H-Index - 242
eISSN - 1521-3765
pISSN - 0947-6539
DOI - 10.1002/chem.201300181
Subject(s) - microreactor , yield (engineering) , flow chemistry , packed bed , chemistry , catalysis , heterogeneous catalysis , flow (mathematics) , biological system , kinetic energy , volumetric flow rate , process engineering , process (computing) , chromatography , thermodynamics , computer science , organic chemistry , mechanics , physics , engineering , biology , quantum mechanics , operating system
The heterogeneous proline‐catalyzed aldol reaction was investigated under continuous‐flow conditions by means of a packed‐bed microreactor. Reaction‐progress kinetic analysis (RPKA) was used in combination with nonlinear chromatography for the interpretation, under synthetically relevant conditions, of important mechanistic aspects of the heterogeneous catalytic process at a molecular level. The information gathered by RPKA and nonlinear chromatography proved to be highly complementary and allowed for the assessment of optimal operating variables. In particular, the determination of the rate‐determining step was pivotal for optimizing the feed composition. On the other hand, the competitive product inhibition was responsible for the unexpected decrease in the reaction yield following an apparently obvious variation in the feed composition. The study was facilitated by a suitable 2D instrumental arrangement for simultaneous flow reaction and online flow‐injection analysis.