التفاصيل البيبلوغرافية
العنوان: |
Assessing the Role of Site Isolation and Compartmentalization in Packed-Bed Flow Reactors for Processes Involving Wolf-and-Lamb Scenarios |
المؤلفون: |
Parijat Borah (1580110), Mauro Fianchini (1955215), Miquel A. Pericàs (1368555) |
سنة النشر: |
2021 |
المجموعة: |
Smithsonian Institution: Digital Repository |
مصطلحات موضوعية: |
Biophysics, Biochemistry, Biotechnology, Environmental Sciences not elsewhere classified, Biological Sciences not elsewhere classified, sequential transformations, tandem processes, flow reactor, packed-bed reactors, Packed-Bed Flow Reactors, sulfonic acid, approach, PBR, MHC, compartmentalization, wolf-and-lamb reactions, Site Isolation, catalyze acetal hydrolysis, rate-limiting step, Knoevenagel condensation, equivalent solutions, DFT study, Wolf-and-Lamb Scenarios, base catalysts, Henry reaction, mesoporous silica-based acid, mesoporous silica-based catalysts, amine sites |
الوصف: |
While catalytic tandem processes in batch involving mutually incompatible catalysts (wolf-and-lamb reactions) can be tackled with different approaches [physical compartmentalization of individual catalytic processes or multifunctional heterogeneous catalysts (MHCs) with catalytic site isolation], no equivalent solutions have been developed to date for the corresponding processes performed in flow with packed-bed reactors (PBRs). To fill this gap, the role of “site isolation” and “compartmentalization” in a flow reactor packed with mesoporous silica-based catalysts, containing sulfonic acid and primary amine sites, to catalyze acetal hydrolysis, followed by C–C bond-forming condensation reactions, such as the Henry reaction or the Knoevenagel condensation, has been studied. The main consequence of the study is that a simple physical mixture of mesoporous silica-based acid and base catalysts efficiently creates site isolation between the incompatible catalytic sites without the need of any additional compartmentalization inside a single PBR. With this simple approach, examples of important reactions of “wolf-and-lamb” type have been performed in continuous flow with very high productivity, with the catalytic system exhibiting high stability, allowing long-time operation without decrease in performance. A DFT study provides an explanation for the experimental observations and sheds light on the significance of compartmentalization in PBR when the rate-limiting step in sequential transformations is characterized by an unfavorable equilibrium constant. |
نوع الوثيقة: |
article in journal/newspaper |
اللغة: |
unknown |
Relation: |
https://figshare.com/articles/journal_contribution/Assessing_the_Role_of_Site_Isolation_and_Compartmentalization_in_Packed-Bed_Flow_Reactors_for_Processes_Involving_Wolf-and-Lamb_Scenarios/14565796 |
DOI: |
10.1021/acscatal.1c00889.s001 |
الاتاحة: |
https://doi.org/10.1021/acscatal.1c00889.s001 |
Rights: |
CC BY-NC 4.0 |
رقم الانضمام: |
edsbas.8DE23A8D |
قاعدة البيانات: |
BASE |