Microfluidic Reactors Based on Rechargeable Catalytic Porous Supports: Heterogeneous Enzymatic Catalysis via Reversible Host–Guest Interactions

León, Alberto Sanz de; Vargas-Alfredo, Nelson; Gallardo, Alberto; Fernández-Mayoralas, Alfonso; Bastida, Ágatha; Muñoz‐Bonilla, Alexandra; Rodríguez‐Hernández, Juan

doi:10.1021/acsami.6b13554

Cited by 19 publications

(7 citation statements)

References 26 publications

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“…The immobilization into the inner surface of wall-coated reactors usually aims at forming uniform monolayers by directed immobilization [12,16,17] or by the controlled formation of thin films [38,39]. However, when the inner reactor area is insufficient, surface coating with nanomaterials (i.e nanoparticles, nanosprings, nanotubes…) [40][41][42][43] and polymers [44] increases the enzyme loadings by 10-15 fold.…”

Section: Introductionmentioning

confidence: 99%

Characterization and evaluation of immobilized enzymes for applications in flow reactors

Bolívar

López‐Gallego

2020

Current Opinion in Green and Sustainable Chemistry

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Section: Introductionmentioning

confidence: 99%

Characterization and evaluation of immobilized enzymes for applications in flow reactors

Bolívar

López‐Gallego

2020

Current Opinion in Green and Sustainable Chemistry

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“…The idea in general is that by combining the high selectivity of enzymes with the efficient fluidics of a microstructured flow reactor, the performance characteristics of certain chemical transformations can be enhanced substantially. Fundamental problem of all microfluidic biocatalysis in continuous flow is, however, that irrespective of the enzyme’s actual use for sample pretreatment, analytical detection, or organic synthesis, the enzyme must be applied in a form that prevents it from being washed away. − , Immobilizing the enzyme on the wall surface of the microchannels presents the most straightforward solution. ,− Doing so, however, demands a strongly integrated development of the microfluidic system considered. The flow channels must be designed to accommodate a suitable amount of active enzyme immobilized on their solid walls because the conversion rate scales directly with that amount. ,,, The contrast to enzyme immobilization in conventional reactors is immediately noted.…”

Section: Introductionmentioning

confidence: 99%

A Spring in Performance: Silica Nanosprings Boost Enzyme Immobilization in Microfluidic Channels

Valikhani

Bolívar

Viefhues

et al. 2017

ACS Appl. Mater. Interfaces

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Enzyme microreactors are important tools of miniaturized analytics and have promising applications in continuous biomanufacturing. A fundamental problem of their design is that plain microchannels without extensive static internals, or packings, offer limited exposed surface area for immobilizing the enzyme. To boost the immobilization in a manner broadly applicable to enzymes, we coated borosilicate microchannels with silica nanosprings and attached the enzyme, sucrose phosphorylase, via a silica-binding module genetically fused to it. We showed with confocal fluorescence microscopy that the enzyme was able to penetrate the ∼70 μm-thick nanospring layer and became distributed uniformly in it. Compared with the plain surface, the activity of immobilized enzyme was enhanced 4.5-fold upon surface coating with nanosprings and further increased up to 10-fold by modifying the surface of the nanosprings with sulfonate groups. Operational stability during continuous-flow biocatalytic synthesis of α-glucose 1-phosphate was improved by a factor of 11 when the microreactor coated with nanosprings was used. More than 85% of the initial conversion rate was retained after 840 reactor cycles performed with a single loading of enzyme. By varying the substrate flow rate, the microreactor performance was conveniently switched between steady states of quantitative product yield (50 mM) and optimum productivity (19 mM min) at a lower product yield of 40%. Surface coating with silica nanosprings thus extends the possibilities for enzyme immobilization in microchannels. It effectively boosts the biocatalytic function of a microstructured reactor limited otherwise by the solid surface available for immobilizing the enzyme.

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“…We wish to emphasize the important interrelationship between STY , k cat , d h , and E imm in defining the performance of a wall‐coated enzyme microreactor. Although there are microreactor studies focusing on increase of E imm or reduction of d h , this aspect has not been addressed.…”

Section: Resultsmentioning

confidence: 99%

Demystifying the Flow: Biocatalytic Reaction Intensification in Microstructured Enzyme Reactors

2018

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Continuous (flow) reactors have drawn a wave of renewed interest in biocatalysis. Many studies find that the flow reactor offers enhanced conversion efficiency. What the reported reaction intensification actually consists in, however, often remains obscure. Here, a canonical microreactor design for heterogeneously catalyzed continuous biotransformations, featuring flow microchannels that contain the enzyme immobilized on their wall surface are examined. Glycosylations by sucrose phosphorylase are used to assess the potential for reaction intensification due to microscale effects. Key variables are identified, and their corresponding relationship equations, to describe, and optimize, the interplay between reaction characteristics, microchannel geometry and reactor operation. The maximum space-time-yield (STY_max) scales directly with the enzyme activity immobilized on the available wall surface. Timescale analysis, comparing the characteristic times of reaction (τ ) and diffusion (τ ) to the mean residence time (τ ), reveals operational conditions for optimum reactor output. Theoretical insight into determinants of microreactor performance is applied to biocatalytic syntheses of α-d-glucose 1-phosphate and α-glucosyl glycerol. Process boundaries for enzyme showing, respectively, high (80 U mg ) and low (4 U mg ) specific activities are thus established and options for process design revealed. Opportunities, and limitations, of the application of principles of microscale flow chemistry to biocatalytic transformations are made evident.

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Microfluidic Reactors Based on Rechargeable Catalytic Porous Supports: Heterogeneous Enzymatic Catalysis via Reversible Host–Guest Interactions

Cited by 19 publications

References 26 publications

Characterization and evaluation of immobilized enzymes for applications in flow reactors

Characterization and evaluation of immobilized enzymes for applications in flow reactors

A Spring in Performance: Silica Nanosprings Boost Enzyme Immobilization in Microfluidic Channels

Demystifying the Flow: Biocatalytic Reaction Intensification in Microstructured Enzyme Reactors

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