Mechanoresponsive and recyclable biocatalytic sponges from enzyme-polymer surfactant conjugates and nanoparticles

Jain, Mehak; Vaze, Rutuja G.; Ugrani, Suraj; Sharma, Kamendra P.

doi:10.1039/c8ra08221a

Cited by 14 publications

(26 citation statements)

References 26 publications

(36 reference statements)

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“…Among the various methodologies which have been developed during the last decades for the immobilization of enzymes on silica surfaces, 1−26 one recently developed method is based on the preparation of dendronized polymer (denpol)–enzyme conjugates. 27−30 The principle of the method is simple.…”

Section: Introductionmentioning

confidence: 99%

Stable Immobilization of Enzymes in a Macro- and Mesoporous Silica Monolith

et al. 2019

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Horseradish peroxidase isoenzyme C (HRP) and Engyodontium album proteinase K (proK) were immobilized inside macro- and mesoporous silica monoliths. Stable immobilization was achieved through simple noncovalent adsorption of conjugates, which were prepared from a polycationic, water-soluble second generation dendronized polymer (denpol) and the enzymes. Conjugates prepared from three denpols with the same type of repeating unit (r.u.), but different average lengths were compared. It was shown that there is no obvious advantage of using denpols with very long chains. Excellent results were achieved with denpols having on average 750 or 1000 r.u. The enzyme-loaded monoliths were tested as flow reactors. Comparison was made with microscopy glass coverslips onto which the conjugates were immobilized and with glass micropipettes containing adsorbed conjugates. High enzyme loading was achieved using the monoliths. Monoliths containing immobilized denpol–HRP conjugates exhibited good operational stability at 25 °C (for at least several hours), and good storage stability at 4 °C (at least for weeks) was demonstrated. Such HRP-containing monoliths were applied as continuous flow reactors for the quantitative determination of hydrogen peroxide in aqueous solution between 1 μM (34 ng/mL) and 50 μM (1.7 μg/mL). Although many methods for immobilizing enzymes on silica surfaces exist, there are only a few approaches with porous silica materials for the development of flow reactors. The work presented is a promising contribution to this field of research toward bioanalytical and biosynthetic applications.

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Section: Introductionmentioning

confidence: 99%

Stable Immobilization of Enzymes in a Macro- and Mesoporous Silica Monolith

et al. 2019

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“…The chromophore substrate 2,2′‐azino‐bis(3‐ethylbenzothiazoline)‐6‐sulfonic acid (ABTS) and Fc were used to analyze the formation of H 2 O 2 in the presence and absence of O 2 . ABTS in the presence of H 2 O 2 is known to change into the chromophore ABTS .+ radical cation, which absorbs at 420 nm while formation of Fc + was analyzed at 630 nm as before using UV/Vis spectroscopy [24, 26] . While in the presence of O 2 , ABTS and Fc converted rapidly into ABTS .+ and Fc + , respectively, on reaction with H 2 O 2 , there was no transformation seen in either case in the of absence of O 2 (SI Figure S2, methods (v)(ii)).…”

Section: Resultsmentioning

confidence: 99%

“…The re‐oxidation behavior was tested for 4 more cycles by adding a fixed 5 m m concentration of d ‐glucose at the end of each cycle (Figure 1 c , inset). We note that cascade reactions of GOx and HRP have been used for the modification of soft matter such as fabrication of bio‐functional liquid crystal droplets, [24] nanoreactor coacervates, [25] mechanoresponsive sponges, [26] and biocatalytic electrodes. [27] The mechanism of the cascade reaction involves oxidation of d ‐glucose by GOx largely aided by its cofactor FAD to form β‐ d ‐gluconate ions and FADH 2 .…”

Section: Resultsmentioning

confidence: 99%

Fuel‐Driven and Enzyme‐Regulated Redox‐Responsive Supramolecular Hydrogels

Jain

Ravoo

2021

Angew Chem Int Ed

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Chemical reaction networks (CRN) embedded in hydrogels can transform responsive materials into complex self‐regulating materials that generate feedback to counter the effect of external stimuli. This study presents hydrogels containing the β‐cyclodextrin (CD) and ferrocene (Fc) host–guest pair as supramolecular crosslinks where redox‐responsive behavior is driven by the enzyme–fuel couples horse radish peroxidase (HRP)–H2O2 and glucose oxidase (GOx)–d‐glucose. The hydrogel can be tuned from a responsive to a self‐regulating supramolecular system by varying the concentration of added reduction fuel d‐glucose. The onset of self‐regulating behavior is due to formation of oxidation fuel in the hydrogel by a cofactor intermediate GOx[FADH2]. UV/Vis spectroscopy, rheology, and kinetic modeling were employed to understand the emergence of out‐of‐equilibrium behavior and reveal the programmable negative feedback response of the hydrogel, including the adaptation of its elastic modulus and its potential as a glucose sensor.

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“…Nützlich ist hier, dass ABTS durch H 2 O 2 zum Radikalkation ABTS .+ oxidiert wird, das eine charakteristische Absorption bei 420 nm aufweist. Dies konnte wie zuvor bei Fc + (630 nm) durch UV/Vis‐Spektroskopie charakterisiert werden [24, 26] . In Anwesenheit von O 2 wurden sowohl ABTS als auch Fc durch H 2 O 2 schnell in ABTS .+ bzw.…”

Section: Ergebnisse Und Diskussionunclassified

Brennstoffbetriebene und enzymregulierte redoxresponsive supramolekulare Hydrogele

Jain

Ravoo

2021

Angewandte Chemie

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In Hydrogele eingebrachte chemische Reaktionsnetzwerke können responsive Materialien zu komplexen, selbstregulierenden Materialien transformieren, die eine Rückkopplung auf externe Stimuli generieren können. Diese Arbeit präsentiert Hydrogele aus dem Wirt‐Gast‐Paar β‐Cyclodextrin und Ferrocen als supramolekulare Vernetzer. Ein redoxresponsives Verhalten des Systems wird induziert durch die Treibstoff‐Enzym‐Paare Meerrettich‐Peroxidase/H2O2 und Glucose‐Oxidase (GOx)/d‐Glucose. Das Hydrogel kann durch Variation der Konzentration des Reduktionstreibstoffs d‐Glucose von einem responsiven zu einem selbstregulierenden supramolekularen System umgewandelt werden. Gestartet wird das selbstregulierende Verhalten durch die Bildung eines Oxidationsmittels innerhalb des Gels durch das Cofaktor‐Intermediat GOx[FADH2]. UV/Vis‐Spektroskopie, Rheologie und kinetische Modellierung wurden angewendet, um dieses Nichtgleichgewichtsverhalten und die Programmierbarkeit der Rückkopplung des Hydrogels, unter anderem die Anpassung des Speichermoduls und die mögliche Anwendung als Glucose‐Sensor, zu beleuchten.

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Mechanoresponsive and recyclable biocatalytic sponges from enzyme-polymer surfactant conjugates and nanoparticles

Abstract: The fabrication of biocatalytic, porous, recyclable, and mechanoresponsive elastic sponge like material is shown from a mixture of core–shell alkaline phosphatase-polymer surfactant bioconjugates and nanoparticles.

Cited by 14 publications

References 26 publications

Stable Immobilization of Enzymes in a Macro- and Mesoporous Silica Monolith

Stable Immobilization of Enzymes in a Macro- and Mesoporous Silica Monolith

Fuel‐Driven and Enzyme‐Regulated Redox‐Responsive Supramolecular Hydrogels

Brennstoffbetriebene und enzymregulierte redoxresponsive supramolekulare Hydrogele

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