scholarly journals Self-Immobilizing Biocatalysts Maximize Space–Time Yields in Flow Reactors

Catalysts ◽  
2019 ◽  
Vol 9 (2) ◽  
pp. 164 ◽  
Author(s):  
Theo Peschke ◽  
Patrick Bitterwolf ◽  
Silla Hansen ◽  
Jannis Gasmi ◽  
Kersten Rabe ◽  
...  
Keyword(s):  
Flow Reactor ◽  
Lactobacillus Brevis ◽  
Packed Bed ◽  
Cascade Reactions ◽  
Space Time ◽  
Flow Reactors ◽  
Great Utility ◽  
Platform Comparison ◽  
Cross Platform ◽  
Coated Surfaces

Maximizing space–time yields (STY) of biocatalytic flow processes is essential for the establishment of a circular biobased economy. We present a comparative study in which different biocatalytic flow reactor concepts were tested with the same enzyme, the (R)-selective alcohol dehydrogenase from Lactobacillus brevis (LbADH), that was used for stereoselective reduction of 5-nitrononane-2,8-dione. The LbADH contained a genetically encoded streptavidin (STV)-binding peptide to enable self-immobilization on STV-coated surfaces. The purified enzyme was immobilized by physisorption or chemisorption as monolayers on the flow channel walls, on magnetic microbeads in a packed-bed format, or as self-assembled all-enzyme hydrogels. Moreover, a multilayer biofilm with cytosolic-expressed LbADH served as a whole-cell biocatalyst. To enable cross-platform comparison, STY values were determined for the various reactor modules. While mono- and multilayer coatings of the reactor surface led to STY < 10, higher productivity was achieved with packed-bed reactors (STY ≈ 100) and the densely packed hydrogels (STY > 450). The latter modules could be operated for prolonged times (>6 days). Given that our approach should be transferable to other enzymes, we anticipate that compartmentalized microfluidic reaction modules equipped with self-immobilizing biocatalysts would be of great utility for numerous biocatalytic and even chemo-enzymatic cascade reactions under continuous flow conditions.

scholarly journals Improving Productivity of Multiphase Flow Aerobic Oxidation Using a Tube-in-Tube Membrane Contactor

Catalysts ◽  
2019 ◽  
Vol 9 (1) ◽  
pp. 95 ◽  
Author(s):  
Michael Burkholder ◽  
Stanley Gilliland ◽  
Adam Luxon ◽  
Christina Tang ◽  
B. Gupton
Keyword(s):  
Flow Reactor ◽  
Aerobic Oxidation ◽  
Flow Chemistry ◽  
Packed Bed ◽  
Space Time ◽  
Catalytic Reactions ◽  
Packed Bed Reactor ◽  
Membrane Contactor ◽  
Flow Reactors ◽  
Space Time Yield

The application of flow reactors in multiphase catalytic reactions represents a promising approach for enhancing the efficiency of this important class of chemical reactions. We developed a simple approach to improve the reactor productivity of multiphase catalytic reactions performed using a flow chemistry unit with a packed bed reactor. Specifically, a tube-in-tube membrane contactor (sparger) integrated in-line with the flow reactor has been successfully applied to the aerobic oxidation of benzyl alcohol to benzaldehyde utilizing a heterogeneous palladium catalyst in the packed bed. We examined the effect of sparger hydrodynamics on reactor productivity quantified by space time yield (STY). Implementation of the sparger, versus segmented flow achieved with the built in gas dosing module (1) increased reactor productivity 4-fold quantified by space time yield while maintaining high selectivity and (2) improved process safety as demonstrated by lower effective operating pressures.

scholarly journals Catalysis-in-a-Box: Robotic Screening of Catalytic Materials in the Time of COVID-19

2020 ◽  
Author(s):  
Gaurav Kumar ◽  
Hannah Bossert ◽  
Daniel McDonald ◽  
Anargyros Chatzidmitriou ◽  
M. Alexander Ardagh ◽  
...  
Keyword(s):  
Flow Reactor ◽  
Low Cost ◽  
Packed Bed ◽  
Reaction Rates ◽  
Laboratory Scale ◽  
Materials Testing ◽  
Kinetic Measurements ◽  
Flow Reactors ◽  
Activation Barriers ◽  
Micro Flow

<p></p><p>The emergence of a viral pandemic has motivated the transition away from traditional, labor-intensive materials testing techniques to new automated approaches without compromising on data quality and at costs viable for academic laboratories. Reported here is the design and implementation of an autonomous micro-flow reactor for catalyst evaluation condensing conventional laboratory-scale analogues within a single gas chromatograph (GC), enabling the control of relevant parameters including reactor temperature and reactant partial pressures directly from the GC. Inquiries into the hydrodynamic behavior, temperature control, and heat/mass transfer were sought to evaluate the efficacy of the micro-flow reactor for kinetic measurements. As a catalyst material screening example, a combination of four Brønsted acid catalyzed probe reactions, namely the dehydration of ethanol, 2-propanol, 1-butanol, and the dehydra-decyclization of 2-methyltetrahydrofuran on a solid acid HZSM-5 (Si/Al 140), were carried out in the temperature range 403-543 K for the measurement of apparent reaction kinetics. Product selectivities, proton-normalized reaction rates, and apparent activation barriers were in agreement with measurements performed on conventional packed bed flow reactors. Furthermore, the developed micro-flow reactor was demonstrated to be about ten-fold cheaper to fabricate than commercial automated laboratory-scale reactor setups and is intended to be used for kinetic investigations in vapor-phase catalytic chemistries, with the key benefits including automation, low cost, and limited experimental equipment instrumentation.</p><p></p>

Catalysis-in-a-Box: A Micro-flow Catalytic Reactor Integrated within a Gas Chromatograph for Automated Kinetic Measurements

2019 ◽  
Author(s):  
Gaurav Kumar ◽  
Hannah Bossert ◽  
Daniel McDonald ◽  
Anargyros Chatzidmitriou ◽  
M. Alexander Ardagh ◽  
...  
Keyword(s):  
Flow Reactor ◽  
Packed Bed ◽  
Reaction Rates ◽  
Gas Chromatograph ◽  
Kinetic Measurements ◽  
Flow Reactors ◽  
Activation Barriers ◽  
Partial Pressures ◽  
Micro Flow ◽  
Kinetic Investigations

<p>The design and implementation of an autonomous micro-flow-reactor condensing conventional laboratory-scale analogues within a single gas chromatograph (GC) is reported, enabling the control of relevant parameters including reactor temperature and reactant partial pressures directly from the GC. Inquiries into the hydrodynamic behavior, temperature control, and heat/mass transfer were sought to evaluate the efficacy of the micro-flow-reactor for kinetic measurements. A combination of four Brønsted acid catalyzed probe reactions, namely the dehydration of ethanol, 2-propanol, 1-butanol, and the dehydra-decyclization of 2-methyltetrahydrofuran on a solid acid HZSM-5 (Si/Al 140), were carried out in the temperature range 403-543 K for the measurement of apparent reaction kinetics. Product selectivities, proton-normalized reaction rates, and apparent activation barriers were found to be in agreement with measurements performed in conventional packed bed flow reactors. The developed micro-flow-reactor is therefore intended to be used for kinetic investigations in vapor-phase catalytic chemistries, with the key benefits including automation and limited experimental equipment instrumentation.</p>

Immobilized Whole Cells as Effective Catalysts for Chiral Alcohol Production

2009 ◽  
Vol 62 (9) ◽  
pp. 1034 ◽  
Author(s):  
Jeck Fei Ng ◽  
Stephan Jaenicke
Keyword(s):  
Flow Reactor ◽  
Batch Reactor ◽  
Enantiomeric Excess ◽  
Lactobacillus Brevis ◽  
Packed Bed ◽  
Alginate Beads ◽  
Packed Bed Reactor ◽  
Process Conditions ◽  
Alcohol Production ◽  
Whole Cells

Recombinant Escherichia coli overexpressing the gene LbADH, which encodes for an alcohol dehydrogenase from Lactobacillus brevis, was successfully transformed and cultured. The cells are able to catalyze the reduction of pro-chiral ketones, e.g. ethyl acetoacetate into R-(–)ethyl hydroxybutyrate (EHB) with high conversion and enantiomeric excess >99%. Immobilizing the whole cells in alginate beads leads to a catalyst with improved stability and ease of handling while maintaining the high activity of the free cells. The whole-cell catalyst was tested in a stirred batch reactor (CSTR) and in a continuously operated packed-bed reactor. An Mg2+ concentration of 2 mM was crucial for maintaining the activity of the biocatalyst. After a partial optimization of the process conditions, a productivity of 1.4 gEHB gwcw–1 h–1 could be maintained in a continuous flow reactor over a prolonged period of time.

scholarly journals Catalysis-in-a-Box: Robotic Screening of Catalytic Materials in the Time of COVID-19

2020 ◽  
Author(s):  
Gaurav Kumar ◽  
Hannah Bossert ◽  
Daniel McDonald ◽  
Anargyros Chatzidmitriou ◽  
M. Alexander Ardagh ◽  
...  
Keyword(s):  
Flow Reactor ◽  
Low Cost ◽  
Packed Bed ◽  
Reaction Rates ◽  
Laboratory Scale ◽  
Materials Testing ◽  
Kinetic Measurements ◽  
Flow Reactors ◽  
Activation Barriers ◽  
Micro Flow

<p></p><p>The emergence of a viral pandemic has motivated the transition away from traditional, labor-intensive materials testing techniques to new automated approaches without compromising on data quality and at costs viable for academic laboratories. Reported here is the design and implementation of an autonomous micro-flow reactor for catalyst evaluation condensing conventional laboratory-scale analogues within a single gas chromatograph (GC), enabling the control of relevant parameters including reactor temperature and reactant partial pressures directly from the GC. Inquiries into the hydrodynamic behavior, temperature control, and heat/mass transfer were sought to evaluate the efficacy of the micro-flow reactor for kinetic measurements. As a catalyst material screening example, a combination of four Brønsted acid catalyzed probe reactions, namely the dehydration of ethanol, 2-propanol, 1-butanol, and the dehydra-decyclization of 2-methyltetrahydrofuran on a solid acid HZSM-5 (Si/Al 140), were carried out in the temperature range 403-543 K for the measurement of apparent reaction kinetics. Product selectivities, proton-normalized reaction rates, and apparent activation barriers were in agreement with measurements performed on conventional packed bed flow reactors. Furthermore, the developed micro-flow reactor was demonstrated to be about ten-fold cheaper to fabricate than commercial automated laboratory-scale reactor setups and is intended to be used for kinetic investigations in vapor-phase catalytic chemistries, with the key benefits including automation, low cost, and limited experimental equipment instrumentation.</p><p></p>

Droplet Factories: Synthesis and Assembly of Silver and Palladium Nanoparticles at the Liquid-Liquid Interface

2019 ◽  
Author(s):  
Suchanuch Sachdev ◽  
Rhushabh Maugi ◽  
Sam Davis ◽  
Scott Doak ◽  
Zhaoxia Zhou ◽  
...  
Keyword(s):  
Iron Oxide ◽  
Reaction Rate ◽  
Tertiary Structure ◽  
Flow Reactor ◽  
Pd Nanoparticles ◽  
Subsequent Removal ◽  
Immiscible Liquids ◽  
Flow Reactors ◽  
Droplet Flow ◽  
One Step

<div>The interface between two immiscible liquids represent an ideal substrate for the assembly of nanomaterials. The defect free surface provides a reproducible support for creating densely packed ordered materials. Here a droplet flow reactor is presented for the synthesis and/ or assembly of nanomaterials at the interface of the emulsion. Each droplet acts as microreactor for a reaction between decamethylferrocene (DmFc) within the hexane and metal salts (Ag+/ Pd2+) in the aqueous phase. The hypothesis was that a spontaneous, interfacial reaction would lead to the assembly of nanomaterials creating a Pickering emulsion. The subsequent removal of the solvents showed how the Ag nanoparticles were trapped at the interface and retain the shape of the droplet, however the Pd nanoparticles were dispersed with no tertiary structure. To further exploit this, a one-step process where the particles are synthesised and then assembled into core-shell materials was proposed. The same reactions were performed in the presence of oleic acid stabilise Iron oxide nanoparticles dispersed within the hexane. It was shown that by changing the reaction rate and ratio between palladium and iron oxide a continuous coating of palladium onto iron oxide microspheres can be created. The same reaction with silver, was unsuccessful and resulted in the silver particles being shed into solution, or incorporated within the iron oxide micro particle. These insights offer a new method and chemistry within flow reactors for the creation of palladium and silver nanoparticles. We use the technique to create metal coated iron oxide nanomaterials but the methodology could be easily transferred to the assembly of other materials.</div><div><br></div>

scholarly journals Towards a Novel Computer-Aided Optimization of Microreactors: Techno-Economic Evaluation of an Immobilized Enzyme System

Symmetry ◽  
2021 ◽  
Vol 13 (3) ◽  
pp. 524
Author(s):  
Philip Pietrek ◽  
Manfred Kraut ◽  
Roland Dittmeyer
Keyword(s):  
Magnetic Beads ◽  
Glucose Dehydrogenase ◽  
Packed Bed ◽  
Detailed Knowledge ◽  
Reaction Conditions ◽  
Flow Reactors ◽  
Continuous Flow Reactors ◽  
Enzyme Cascades ◽  
And Control ◽  
Physical And Chemical

Immobilized multi-enzyme cascades are increasingly used in microfluidic devices. In particular, their application in continuous flow reactors shows great potential, utilizing the benefits of reusability and control of the reaction conditions. However, capitalizing on this potential is challenging and requires detailed knowledge of the investigated system. Here, we show the application of computational methods for optimization with multi-level reactor design (MLRD) methodology based on the underlying physical and chemical processes. We optimize a stereoselective reduction of a diketone catalyzed by ketoreductase (Gre2) and Nicotinamidadenindinukleotidphosphat (NADPH) cofactor regeneration with glucose dehydrogenase (GDH). Both enzymes are separately immobilized on magnetic beads forming a packed bed within the microreactor. We derive optimal reactor feed concentrations and enzyme ratios for enhanced performance and a basic economic model in order to maximize the techno-economic performance (TEP) for the first reduction of 5-nitrononane-2,8-dione.

scholarly journals Diels–Alder reactions of myrcene using intensified continuous-flow reactors

2017 ◽  
Vol 13 ◽  
pp. 120-126 ◽  
Author(s):  
Christian H Hornung ◽  
Miguel Á Álvarez-Diéguez ◽  
Thomas M Kohl ◽  
John Tsanaktsidis
Keyword(s):  
Continuous Flow ◽  
Flow Reactor ◽  
Scale Up ◽  
Reaction Times ◽  
Alder Reaction ◽  
Diels Alder ◽  
Flow Reactors ◽  
Diels Alder Reaction ◽  
Naturally Occurring ◽  
Continuous Flow Reactors

This work describes the Diels–Alder reaction of the naturally occurring substituted butadiene, myrcene, with a range of different naturally occurring and synthetic dienophiles. The synthesis of the Diels–Alder adduct from myrcene and acrylic acid, containing surfactant properties, was scaled-up in a plate-type continuous-flow reactor with a volume of 105 mL to a throughput of 2.79 kg of the final product per day. This continuous-flow approach provides a facile alternative scale-up route to conventional batch processing, and it helps to intensify the synthesis protocol by applying higher reaction temperatures and shorter reaction times.

scholarly journals Nitrate radical generation via continuous generation of dinitrogen pentoxide in a laminar flow reactor coupled to an oxidation flow reactor

2020 ◽  
Author(s):  
Andrew T. Lambe ◽  
Ezra C. Wood ◽  
Jordan E. Krechmer ◽  
Francesca Majluf ◽  
Leah R. Williams ◽  
...  
Keyword(s):  
Laminar Flow ◽  
Flow Reactor ◽  
Nitrate Radical ◽  
Peroxy Radicals ◽  
Flow Reactors ◽  
Dinitrogen Pentoxide ◽  
Oxidative Aging ◽  
Chemical Systems ◽  
Alkyl Radicals ◽  
Aerosol Mass

Abstract. Oxidation flow reactors (OFRs) are an emerging tool for studying the formation and oxidative aging of organic aerosols and other applications. The majority of OFR studies to date involved generation of the hydroxyl radical (OH) to mimic daytime oxidative aging processes. On the other hand, use of the nitrate radical (NO3) in modern OFRs to mimic nighttime oxidative aging processes has been limited due to the complexity of conventional techniques that are used to generate NO3. Here, we present a new method that uses a laminar flow reactor (LFR) to continuously generate dinitrogen pentoxide (N2O5) in the gas phase at room temperature from the NO2 + O3 and NO2 + NO3 reactions. The N2O5 is then injected into a dark Potential Aerosol Mass OFR and decomposes to generate NO3; hereafter, this method is referred to as OFR-iN2O5 (i = injected). To assess the applicability of the OFR-iN2O5 method towards different chemical systems, we present experimental and model characterization of the integrated NO3 exposure, NO3:O3, NO2:NO3, and NO2:O2 as a function of LFR and OFR conditions. These parameters were used to investigate the fate of representative organic peroxy radicals (RO2) and aromatic alkyl radicals generated from volatile organic compound (VOC) + NO3 reactions, and VOCs that are reactive towards both O3 and NO3. Finally, we demonstrate the OFR-iN2O5 method by generating and characterizing secondary organic aerosol from the β-pinene + NO3 reaction.

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