Halloysite Clay Nanotubes for Enzyme Immobilization

Tully, Joshua; Yendluri, Raghuvara; Lvov, Yuri

doi:10.1021/acs.biomac.5b01542

Title: Halloysite Clay Nanotubes for Enzyme Immobilization

Abstract

Halloysite clay is an aluminosilicate nanotube formed by rolling flat sheets of kaolinite clay. They have a 15 nm lumen, 50–70 nm external diameter, length of 0.5–1 μm, and different inside/outside chemistry. Due to these nanoscale properties, they are used for loading, storage, and controlled release of active chemical agents, including anticorrosions, biocides, and drugs. Here, we studied the immobilization in halloysite of laccase, glucose oxidase, and lipase. Overall, negatively charged proteins taken above their isoelectric points were mostly loaded into the positively charged tube’s lumen. Typical tube loading with proteins was 6–7 wt % from which one-third was released in 5–10 h and the other two-thirds remained, providing enhanced biocatalysis in nanoconfined conditions. Immobilized lipase showed enhanced stability at acidic pH, and the optimum pH shifted to more alkaline pH. Immobilized laccase was more stable with respect to time, and immobilized glucose oxidase showed retention of enzymatic activity up to 70 °C, whereas the native sample was inactive.

Authors:

Tully, Joshua ^[1]; Yendluri, Raghuvara ^[1]; Lvov, Yuri ^[2]

Louisiana Tech Univ., Ruston, LA (United States)
Louisiana Tech Univ., Ruston, LA (United States); Ural Federal Univ., Ekaterinburg (Russia)

Publication Date:: Wed Dec 23 00:00:00 EST 2015

Research Org.:: Louisiana State Univ., Baton Rouge, LA (United States)

Sponsoring Org.:: USDOE Office of Science (SC), Basic Energy Sciences (BES); Russian Science Foundation; USEPA

OSTI Identifier:: 1673765

Grant/Contract Number:: SC0012432; 15-12-20021; 9177240

Resource Type:: Accepted Manuscript

Journal Name:: Biomacromolecules

Additional Journal Information:: Journal Volume: 17; Journal Issue: 2; Journal ID: ISSN 1525-7797

Publisher:: American Chemical Society

Country of Publication:: United States

Language:: English

Subject:: 75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; Peptides and proteins; Nanotubes; Adsorption; Immobilization; Thermogravimetric analysis

Citation Formats


                    Tully, Joshua, Yendluri, Raghuvara, and Lvov, Yuri. Halloysite Clay Nanotubes for Enzyme Immobilization.  United States: N. p., 2015. 
Web.  doi:10.1021/acs.biomac.5b01542.

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                    Tully, Joshua, Yendluri, Raghuvara, & Lvov, Yuri. Halloysite Clay Nanotubes for Enzyme Immobilization.  United States.  https://doi.org/10.1021/acs.biomac.5b01542

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                    Tully, Joshua, Yendluri, Raghuvara, and Lvov, Yuri. Wed .  
"Halloysite Clay Nanotubes for Enzyme Immobilization".  United States.  https://doi.org/10.1021/acs.biomac.5b01542.  https://www.osti.gov/servlets/purl/1673765.

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@article{osti_1673765,

  title        = {Halloysite Clay Nanotubes for Enzyme Immobilization},

  author       = {Tully, Joshua and Yendluri, Raghuvara and Lvov, Yuri},

  abstractNote = {Halloysite clay is an aluminosilicate nanotube formed by rolling flat sheets of kaolinite clay. They have a 15 nm lumen, 50–70 nm external diameter, length of 0.5–1 μm, and different inside/outside chemistry. Due to these nanoscale properties, they are used for loading, storage, and controlled release of active chemical agents, including anticorrosions, biocides, and drugs. Here, we studied the immobilization in halloysite of laccase, glucose oxidase, and lipase. Overall, negatively charged proteins taken above their isoelectric points were mostly loaded into the positively charged tube’s lumen. Typical tube loading with proteins was 6–7 wt % from which one-third was released in 5–10 h and the other two-thirds remained, providing enhanced biocatalysis in nanoconfined conditions. Immobilized lipase showed enhanced stability at acidic pH, and the optimum pH shifted to more alkaline pH. Immobilized laccase was more stable with respect to time, and immobilized glucose oxidase showed retention of enzymatic activity up to 70 °C, whereas the native sample was inactive.},

  doi          = {10.1021/acs.biomac.5b01542},

  journal      = {Biomacromolecules},

  number       = 2,

  volume       = 17,

  place        = {United States},

  year         = {Wed Dec 23 00:00:00 EST 2015},

  month        = {Wed Dec 23 00:00:00 EST 2015}

}

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Halloysite Clay Nanotubes as Carriers for Curcumin: Characterization and Application

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Halloysite is a nanostructured clay mineral with hollow tubular structure, which has recently found an important role as delivery system for drugs or other active molecules. One of these is curcumin, main constituent in the rhizome of the plant Curcuma Longa, with a series of useful pharmacological activities, hindered by its poor bioavalaibility and solubility in water. In this study, Halloysite clay nanotubes (HNTs) were characterized in terms of both structure and biocompatibility and they were used for curcumin delivery to cancer cells. The performed 3-(4, 5-dimethythiazol-2-yl)-2, 5-diphenyl-tetrazolium bromide (MTT) assay showed that HNTs have a high biocompatibility, also whenmore »« less
https://doi.org/10.1109/tnano.2016.2524072

Full Text Available
Controlling the release of active compounds from the inorganic carrier halloysite

Journal Article Tescione, F. ; Buonocore, G. G. ; Stanzione, M. ; ... - AIP Conference Proceedings

Halloysite (HNTs), a natural material characterized by a nanotube structure, has been used as an inorganic carrier of active compounds in several applications from medicine to anticorrosion coatings. In this present work, vanillin (VAN) used as a antimicrobial model, has been encapsulated within HNTs for exploiting its applicability in the active food packaging sector. The molecule release rate has been controlled by crosslinking at the tube ends the loaded vanillin with copper ions, thus producing a stopper network. The vanillin-loaded HNTs were characterized using transmission electron microscopy (TEM), Fourier transform infrared (FTIR) spectroscopy and thermo gravimetric analysis. The antimicrobial releasemore »« less
https://doi.org/10.1063/1.4876874

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Title: Halloysite Clay Nanotubes for Enzyme Immobilization

Abstract

Citation Formats

A relationship between protein stability and protein function. journal, January 1995

Protein Adsorption onto Silica Nanoparticles: Conformational Changes Depend on the Particles' Curvature and the Protein Stability journal, November 2004

Zeolite inorganic supports for BSA immobilization: Comparative study of several zeolite crystals and composite membranes journal, March 2007

Halloysite clay minerals — a review journal, December 2005

Halloysite Nanotubes as Biomimetic Nanoreactors journal, May 2005

Facile Fabrication of Flowerlike Natural Nanotube/Layered Double Hydroxide Composites as Effective Carrier for Lysozyme Immobilization journal, May 2015

Immobilization of enzyme biocatalyst on natural halloysite nanotubes journal, December 2010

Chitosan–halloysite hybrid-nanotubes: Horseradish peroxidase immobilization and applications in phenol removal journal, January 2013

Cross-Linked Enzyme Aggregates: A Simple and Effective Method for the Immobilization of Penicillin Acylase journal, May 2000

Biodiesel production from waste oils by using lipase immobilized on hydrotalcite and zeolites journal, November 2007

Adsorption of Proteins to Hydrophobic Sites on Mixed Self-Assembled Monolayers † journal, March 2003

Interfacial adsorption of lipases on very hydrophobic support (octadecyl–Sepabeads): immobilization, hyperactivation and stabilization of the open form of lipases journal, December 2002

Simplified para-nitrophenyl palmitate assay for lipases and esterases journal, December 2002

Halloysite Clay Nanotubes for Resveratrol Delivery to Cancer Cells: Halloysite Clay Nanotubes for Resveratrol Delivery to Cancer Cells journal, August 2012

Selective fabrication of iron oxide particles in halloysite lumen journal, February 2015

Clay nanotube encapsulation for functional biocomposites journal, May 2014

Surface Modification of Halloysite Nanotubes with Dopamine for Enzyme Immobilization journal, October 2013

Protein adsorption to polymer particles: Role of surface properties journal, February 1987

Sorption and immobilization of cellulase on silicate clay minerals journal, October 2005

Functional polymer–clay nanotube composites with sustained release of chemical agents journal, October 2013

Use of coated microtubular halloysite for the sustained release of diltiazem hydrochloride and propranolol hydrochloride journal, March 2003

Comparative protein adsorption in model systems journal, October 1990

Natural Nanotube-Based Biomimetic Porous Microspheres for Significantly Enhanced Biomolecule Immobilization journal, August 2013

Hydrophobically Modified Halloysite Nanotubes as Reverse Micelles for Water-in-Oil Emulsion journal, July 2015

Newly emerging applications of halloysite nanotubes: a review: Applications of halloysite nanotubes journal, January 2010

Size and Shape of Protein Molecules at the Nanometer Level Determined by Sedimentation, Gel Filtration, and Electron Microscopy journal, May 2009

Enhanced pH and thermal stabilities of invertase immobilized on montmorillonite K-10 journal, March 2006

A Stable Nonfluorescent Derivative of Resorufin for the Fluorometric Determination of Trace Hydrogen Peroxide: Applications in Detecting the Activity of Phagocyte NADPH Oxidase and Other Oxidases journal, November 1997

UniProt: a hub for protein information journal, October 2014

Recent advance in research on halloysite nanotubes-polymer nanocomposite journal, August 2014

Self-assembly of clay nanotubes on hair surface for medical and cosmetic formulations journal, January 2018

Cu(CH3CN)4PF6 immobilized on halloysite as efficient heterogeneous catalyst for oxidation of allylic C–H bonds in olefins under mild reaction condition journal, January 2019

Bio-interfactants as double-sided tapes for graphene oxide journal, January 2019

Recent Advances on Surface Modification of Halloysite Nanotubes for Multifunctional Applications journal, November 2017

Nanoarchitectonics meets cell surface engineering: shape recognition of human cells by halloysite-doped silica cell imprints journal, January 2019

Loading of halloysite nanotubes with BSA, α -Lac and β -Lg: a Fourier transform infrared spectroscopic and thermogravimetric study journal, December 2016

Palladated halloysite hybridized with photo-polymerized hydrogel in the presence of cyclodextrin: An efficient catalytic system benefiting from nanoreactor concept: Pd/halloysite hybridized with hydrogel journal, January 2019

The Use of Some Clay Minerals as Natural Resources for Drug Carrier Applications journal, October 2018

Photoluminescent hybrid nanomaterials from modified halloysite nanotubes journal, January 2018

Au–Ag and Pt–Ag bimetallic nanoparticles@halloysite nanotubes: morphological modulation, improvement of thermal stability and catalytic performance journal, January 2018

Chemical modification of halloysite nanotubes for controlled loading and release journal, January 2018

Multicomponent bionanocomposites based on clay nanoarchitectures for electrochemical devices journal, January 2019

A review on innovations in polymeric nanocomposite packaging materials and electrical sensors for food and agriculture journal, May 2019

Efficient synthesis of vitamin A palmitate in nonaqueous medium using self-assembled lipase TLL@apatite hybrid nanoflowers by mimetic biomineralization text, January 2018

Covalently modified halloysite clay nanotubes: synthesis, properties, biological and medical applications journal, January 2017

Gold nanoparticles stabilized by modified halloysite nanotubes for catalytic applications: A flow system based on Au supported on HNT for catalytic applications journal, December 2018

Efficient synthesis of vitamin A palmitate in nonaqueous medium using self-assembled lipase TLL@apatite hybrid nanoflowers by mimetic biomineralization text, January 2018

Recent Advances on Surface Modification of Halloysite Nanotubes for Multifunctional Applications posted_content, October 2017

Recent Advances on Surface Modification of Halloysite Nanotubes for Multifunctional Applications posted_content, October 2017

Halloysite Nanotubes for Cleaning, Consolidation and Protection journal, January 2018

Biomedical potential of clay nanotube formulations and their toxicity assessment journal, September 2019

Palladium nanoparticles immobilized on halloysite nanotubes covered by a multilayer network for catalytic applications journal, January 2018

Hybrid supramolecular gels of Fmoc-F/halloysite nanotubes: systems for sustained release of camptothecin journal, January 2017

A facile one-step grafting of polyphosphonium onto halloysite nanotubes initiated by Ce( iv ) journal, January 2019

Recently emerging advancements in halloysite nanotubes polymer nanocomposites journal, October 2018

CuI-functionalized halloysite nanoclay as an efficient heterogeneous catalyst for promoting click reactions: Combination of experimental and computational chemistry text, January 2022

Functional biohybrid materials based on halloysite, sepiolite and cellulose nanofibers for health applications journal, January 2020

Clay-based drug-delivery systems: what does the future hold? journal, July 2017

Mesoporous inorganic nanoscale particles for drug adsorption and controlled release journal, March 2018

CuI-functionalized halloysite nanoclay as an efficient heterogeneous catalyst for promoting click reactions: Combination of experimental and computational chemistry: CuI@ functionalized halloysite nanoclay for promoting click reaction journal, April 2018

Functionality of chitosan‐halloysite nanocomposite films for sustained delivery of antibiotics: The effect of chitosan molar mass journal, August 2019

Halloysite nanotube-based electrospun ceramic nanofibre mat: a novel support for zeolite membranes journal, December 2016

Current Status of Nanoclay Phytotoxicity book, January 2018

Efficient synthesis of vitamin A palmitate in nonaqueous medium using self-assembled lipase TLL@apatite hybrid nanoflowers by mimetic biomineralization journal, October 2018

Organo-Clay Nanomaterials Based on Halloysite and Cyclodextrin as Carriers for Polyphenolic Compounds journal, November 2018

Halloysite Nanotubes: Controlled Access and Release by Smart Gates journal, July 2017

Selective adsorption of oppositely charged PNIPAAM on halloysite surfaces: a route to thermo-responsive nanocarriers journal, June 2018

Binase Immobilized on Halloysite Nanotubes Exerts Enhanced Cytotoxicity toward Human Colon Adenocarcinoma Cells journal, September 2017

The Use of Some Clay Minerals as Natural Resources for Drug Carrier Applications journal, October 2018

Organo-Clay Nanomaterials Based on Halloysite and Cyclodextrin as Carriers for Polyphenolic Compounds journal, November 2018

Antimicrobial Membranes of Bio-Based PA 11 and HNTs Filled with Lysozyme Obtained by an Electrospinning Process journal, March 2018

Advances in Halloysite Nanotubes–Polysaccharide Nanocomposite Preparation and Applications journal, June 2019

Multicomponent bionanocomposites based on clay nanoarchitectures for electrochemical devices journal, January 2019

Nanoarchitectonics meets cell surface engineering: shape recognition of human cells by halloysite-doped silica cell imprints journal, January 2019

A relationship between protein stability and protein function.
journal, January 1995

Protein Adsorption onto Silica Nanoparticles: Conformational Changes Depend on the Particles' Curvature and the Protein Stability
journal, November 2004

Zeolite inorganic supports for BSA immobilization: Comparative study of several zeolite crystals and composite membranes
journal, March 2007

Halloysite clay minerals — a review
journal, December 2005

Halloysite Nanotubes as Biomimetic Nanoreactors
journal, May 2005

Facile Fabrication of Flowerlike Natural Nanotube/Layered Double Hydroxide Composites as Effective Carrier for Lysozyme Immobilization
journal, May 2015

Immobilization of enzyme biocatalyst on natural halloysite nanotubes
journal, December 2010

Chitosan–halloysite hybrid-nanotubes: Horseradish peroxidase immobilization and applications in phenol removal
journal, January 2013

Cross-Linked Enzyme Aggregates: A Simple and Effective Method for the Immobilization of Penicillin Acylase
journal, May 2000

Biodiesel production from waste oils by using lipase immobilized on hydrotalcite and zeolites
journal, November 2007

Adsorption of Proteins to Hydrophobic Sites on Mixed Self-Assembled Monolayers ^†
journal, March 2003

Interfacial adsorption of lipases on very hydrophobic support (octadecyl–Sepabeads): immobilization, hyperactivation and stabilization of the open form of lipases
journal, December 2002

Simplified para-nitrophenyl palmitate assay for lipases and esterases
journal, December 2002

Halloysite Clay Nanotubes for Resveratrol Delivery to Cancer Cells: Halloysite Clay Nanotubes for Resveratrol Delivery to Cancer Cells
journal, August 2012

Selective fabrication of iron oxide particles in halloysite lumen
journal, February 2015

Clay nanotube encapsulation for functional biocomposites
journal, May 2014

Surface Modification of Halloysite Nanotubes with Dopamine for Enzyme Immobilization
journal, October 2013

Protein adsorption to polymer particles: Role of surface properties
journal, February 1987

Sorption and immobilization of cellulase on silicate clay minerals
journal, October 2005

Functional polymer–clay nanotube composites with sustained release of chemical agents
journal, October 2013

Use of coated microtubular halloysite for the sustained release of diltiazem hydrochloride and propranolol hydrochloride
journal, March 2003

Comparative protein adsorption in model systems
journal, October 1990

Natural Nanotube-Based Biomimetic Porous Microspheres for Significantly Enhanced Biomolecule Immobilization
journal, August 2013

Hydrophobically Modified Halloysite Nanotubes as Reverse Micelles for Water-in-Oil Emulsion
journal, July 2015

Newly emerging applications of halloysite nanotubes: a review: Applications of halloysite nanotubes
journal, January 2010

Size and Shape of Protein Molecules at the Nanometer Level Determined by Sedimentation, Gel Filtration, and Electron Microscopy
journal, May 2009

Enhanced pH and thermal stabilities of invertase immobilized on montmorillonite K-10
journal, March 2006

A Stable Nonfluorescent Derivative of Resorufin for the Fluorometric Determination of Trace Hydrogen Peroxide: Applications in Detecting the Activity of Phagocyte NADPH Oxidase and Other Oxidases
journal, November 1997

UniProt: a hub for protein information
journal, October 2014

Recent advance in research on halloysite nanotubes-polymer nanocomposite
journal, August 2014

Self-assembly of clay nanotubes on hair surface for medical and cosmetic formulations
journal, January 2018

Cu(CH3CN)4PF6 immobilized on halloysite as efficient heterogeneous catalyst for oxidation of allylic C–H bonds in olefins under mild reaction condition
journal, January 2019

Bio-interfactants as double-sided tapes for graphene oxide
journal, January 2019

Recent Advances on Surface Modification of Halloysite Nanotubes for Multifunctional Applications
journal, November 2017

Nanoarchitectonics meets cell surface engineering: shape recognition of human cells by halloysite-doped silica cell imprints
journal, January 2019

Loading of halloysite nanotubes with BSA, α -Lac and β -Lg: a Fourier transform infrared spectroscopic and thermogravimetric study
journal, December 2016

Palladated halloysite hybridized with photo-polymerized hydrogel in the presence of cyclodextrin: An efficient catalytic system benefiting from nanoreactor concept: Pd/halloysite hybridized with hydrogel
journal, January 2019

The Use of Some Clay Minerals as Natural Resources for Drug Carrier Applications
journal, October 2018

Photoluminescent hybrid nanomaterials from modified halloysite nanotubes
journal, January 2018

Au–Ag and Pt–Ag bimetallic nanoparticles@halloysite nanotubes: morphological modulation, improvement of thermal stability and catalytic performance
journal, January 2018

Chemical modification of halloysite nanotubes for controlled loading and release
journal, January 2018

Multicomponent bionanocomposites based on clay nanoarchitectures for electrochemical devices
journal, January 2019

A review on innovations in polymeric nanocomposite packaging materials and electrical sensors for food and agriculture
journal, May 2019

Efficient synthesis of vitamin A palmitate in nonaqueous medium using self-assembled lipase TLL@apatite hybrid nanoflowers by mimetic biomineralization
text, January 2018

Covalently modified halloysite clay nanotubes: synthesis, properties, biological and medical applications
journal, January 2017

Gold nanoparticles stabilized by modified halloysite nanotubes for catalytic applications: A flow system based on Au supported on HNT for catalytic applications
journal, December 2018

Efficient synthesis of vitamin A palmitate in nonaqueous medium using self-assembled lipase TLL@apatite hybrid nanoflowers by mimetic biomineralization
text, January 2018

Recent Advances on Surface Modification of Halloysite Nanotubes for Multifunctional Applications
posted_content, October 2017

Recent Advances on Surface Modification of Halloysite Nanotubes for Multifunctional Applications
posted_content, October 2017

Halloysite Nanotubes for Cleaning, Consolidation and Protection
journal, January 2018

Biomedical potential of clay nanotube formulations and their toxicity assessment
journal, September 2019

Palladium nanoparticles immobilized on halloysite nanotubes covered by a multilayer network for catalytic applications
journal, January 2018

Hybrid supramolecular gels of Fmoc-F/halloysite nanotubes: systems for sustained release of camptothecin
journal, January 2017

A facile one-step grafting of polyphosphonium onto halloysite nanotubes initiated by Ce( iv )
journal, January 2019

Recently emerging advancements in halloysite nanotubes polymer nanocomposites
journal, October 2018

CuI-functionalized halloysite nanoclay as an efficient heterogeneous catalyst for promoting click reactions: Combination of experimental and computational chemistry
text, January 2022

Functional biohybrid materials based on halloysite, sepiolite and cellulose nanofibers for health applications
journal, January 2020

Clay-based drug-delivery systems: what does the future hold?
journal, July 2017

Mesoporous inorganic nanoscale particles for drug adsorption and controlled release
journal, March 2018

CuI-functionalized halloysite nanoclay as an efficient heterogeneous catalyst for promoting click reactions: Combination of experimental and computational chemistry: CuI@ functionalized halloysite nanoclay for promoting click reaction
journal, April 2018

Functionality of chitosan‐halloysite nanocomposite films for sustained delivery of antibiotics: The effect of chitosan molar mass
journal, August 2019

Halloysite nanotube-based electrospun ceramic nanofibre mat: a novel support for zeolite membranes
journal, December 2016

Current Status of Nanoclay Phytotoxicity
book, January 2018

Efficient synthesis of vitamin A palmitate in nonaqueous medium using self-assembled lipase TLL@apatite hybrid nanoflowers by mimetic biomineralization
journal, October 2018

Organo-Clay Nanomaterials Based on Halloysite and Cyclodextrin as Carriers for Polyphenolic Compounds
journal, November 2018

Halloysite Nanotubes: Controlled Access and Release by Smart Gates
journal, July 2017

Selective adsorption of oppositely charged PNIPAAM on halloysite surfaces: a route to thermo-responsive nanocarriers
journal, June 2018

Binase Immobilized on Halloysite Nanotubes Exerts Enhanced Cytotoxicity toward Human Colon Adenocarcinoma Cells
journal, September 2017

The Use of Some Clay Minerals as Natural Resources for Drug Carrier Applications
journal, October 2018

Organo-Clay Nanomaterials Based on Halloysite and Cyclodextrin as Carriers for Polyphenolic Compounds
journal, November 2018

Antimicrobial Membranes of Bio-Based PA 11 and HNTs Filled with Lysozyme Obtained by an Electrospinning Process
journal, March 2018

Advances in Halloysite Nanotubes–Polysaccharide Nanocomposite Preparation and Applications
journal, June 2019

Multicomponent bionanocomposites based on clay nanoarchitectures for electrochemical devices
journal, January 2019

Nanoarchitectonics meets cell surface engineering: shape recognition of human cells by halloysite-doped silica cell imprints
journal, January 2019