Kinetics of temperature response of PEO-b-PNIPAM-b-PAA triblock terpolymer aggregates and of their complexes with lysozyme

Papagiannopoulos, Aristeidis; Meristoudi, Anastasia; Hong, Kunlun; Pispas, Stergios

doi:10.1016/j.polymer.2015.12.023

Title: Kinetics of temperature response of PEO-b-PNIPAM-b-PAA triblock terpolymer aggregates and of their complexes with lysozyme

Abstract

We present the kinetics of temperature response of a PEO-b-PNIPAM-b-PAA triblock terpolymer and of its complexes with lysozyme in aqueous solution. It is found that during the coil-to-globule transition of PNIPAM new bonds within the polymer aggregates are created, making the transition of the aggregates partially irreversible. This effect is also found for the protein loaded PEO-b-PNIPAM-b-PAA aggregates whereas in this case protein globules appear to enhance the formation of bonds, making the transition totally irreversible. The internal dynamics of both aggregates and complexes are “frozen” once the temperature is increased upon PINIPAM's LCST in water and remain so even when the temperature drops below LCST. As a result, we investigate the complexation kinetics of lysozyme and PEO-b-PNIPAM-b-PAA and observe that it occurs in two stages, one where protein globules adsorb on single pre-formed aggregates and one where protein globules cause inter-aggregate clustering.

Authors:

Papagiannopoulos, Aristeidis ^[1]; Meristoudi, Anastasia ^[1]; Hong, Kunlun ^[2]; Pispas, Stergios ^[1]

National Hellenic Research Foundation, Athens (Greece)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)

Publication Date:: Fri Dec 18 00:00:00 EST 2015

Research Org.:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Org.:: USDOE Office of Science (SC)

OSTI Identifier:: 1237639

Grant/Contract Number:: AC05-00OR22725

Resource Type:: Accepted Manuscript

Journal Name:: Polymer

Additional Journal Information:: Journal Volume: 83; Journal Issue: C; Journal ID: ISSN 0032-3861

Publisher:: Elsevier

Country of Publication:: United States

Language:: English

Subject:: 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; thermoresponsive polymers; protein complexation; kinetics

Citation Formats


                    Papagiannopoulos, Aristeidis, Meristoudi, Anastasia, Hong, Kunlun, and Pispas, Stergios. Kinetics of temperature response of PEO-b-PNIPAM-b-PAA triblock terpolymer aggregates and of their complexes with lysozyme.  United States: N. p., 2015. 
Web.  doi:10.1016/j.polymer.2015.12.023.

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                    Papagiannopoulos, Aristeidis, Meristoudi, Anastasia, Hong, Kunlun, & Pispas, Stergios. Kinetics of temperature response of PEO-b-PNIPAM-b-PAA triblock terpolymer aggregates and of their complexes with lysozyme.  United States.  https://doi.org/10.1016/j.polymer.2015.12.023

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                    Papagiannopoulos, Aristeidis, Meristoudi, Anastasia, Hong, Kunlun, and Pispas, Stergios. Fri .  
"Kinetics of temperature response of PEO-b-PNIPAM-b-PAA triblock terpolymer aggregates and of their complexes with lysozyme".  United States.  https://doi.org/10.1016/j.polymer.2015.12.023.  https://www.osti.gov/servlets/purl/1237639.

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@article{osti_1237639,

  title        = {Kinetics of temperature response of PEO-b-PNIPAM-b-PAA triblock terpolymer aggregates and of their complexes with lysozyme},

  author       = {Papagiannopoulos, Aristeidis and Meristoudi, Anastasia and Hong, Kunlun and Pispas, Stergios},

  abstractNote = {We present the kinetics of temperature response of a PEO-b-PNIPAM-b-PAA triblock terpolymer and of its complexes with lysozyme in aqueous solution. It is found that during the coil-to-globule transition of PNIPAM new bonds within the polymer aggregates are created, making the transition of the aggregates partially irreversible. This effect is also found for the protein loaded PEO-b-PNIPAM-b-PAA aggregates whereas in this case protein globules appear to enhance the formation of bonds, making the transition totally irreversible. The internal dynamics of both aggregates and complexes are “frozen” once the temperature is increased upon PINIPAM's LCST in water and remain so even when the temperature drops below LCST. As a result, we investigate the complexation kinetics of lysozyme and PEO-b-PNIPAM-b-PAA and observe that it occurs in two stages, one where protein globules adsorb on single pre-formed aggregates and one where protein globules cause inter-aggregate clustering.},

  doi          = {10.1016/j.polymer.2015.12.023},

  journal      = {Polymer},

  number       = C,

  volume       = 83,

  place        = {United States},

  year         = {Fri Dec 18 00:00:00 EST 2015},

  month        = {Fri Dec 18 00:00:00 EST 2015}

}

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Works referencing / citing this record:

Formation of complexes in aqueous solutions of amphiphilic triblock polyelectrolytes of different topologies and an oppositely charged protein
journal, January 2018

Papagiannopoulos, Aristeidis; Karayianni, Maria; Pispas, Stergios
Soft Matter, Vol. 14, Issue 15
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Title: Kinetics of temperature response of PEO-b-PNIPAM-b-PAA triblock terpolymer aggregates and of their complexes with lysozyme

Abstract

Citation Formats

Emerging applications of stimuli-responsive polymer materials journal, January 2010

Structure and design of polymeric surfactant-based drug delivery systems journal, June 2001

Spherical polyelectrolyte brushes journal, October 2007

Self-Cross-Linked Polymer Nanogels: A Versatile Nanoscopic Drug Delivery Platform journal, December 2010

Thermoresponsive hydrogels in biomedical applications journal, January 2008

Hydrogels in drug delivery: Progress and challenges journal, April 2008

Microgels as Nanoreactors: Applications in Catalysis book, January 2010

Reduction and temperature dual-responsive crosslinked polymersomes for targeted intracellular protein delivery journal, January 2011

Morphological transitions in aggregates of thermosensitive poly(ethylene oxide)- b -poly( N -isopropylacrylamide) block copolymers prepared via RAFT polymerization: Morphological Transitions in PEO- b -PNIPAM journal, July 2009

Living Radical Polymerization by the RAFT Process - A Second Update journal, January 2009

Micellar and fractal aggregates formed by two triblock terpolymers with different arrangements of one charged, one neutral hydrophilic and one hydrophobic block journal, April 2015

Light Scattering by Fractal Aggregates: A Review journal, January 2001

Dynamic light scattering study of internal motions of polymer coils in dilute solution journal, December 1991

Asymptotic behavior and long-range interactions in aqueous solutions of poly(ethylene oxide) journal, October 1991

Characterization of Poly(N-isopropylmethacrylamide) in Water journal, December 1990

Structure of Micelles of Poly( n -butyl acrylate)- block -poly(acrylic acid) Diblock Copolymers in Aqueous Solution journal, June 2007

Thermoresponsive transition of a PEO-b-PNIPAM copolymer: From hierarchical aggregates to well defined ellipsoidal vesicles journal, November 2013

Thermoresponsive aggregation of PS–PNIPAM–PS triblock copolymer: A combined study of light scattering and small angle neutron scattering journal, July 2014

Interchain Hydrogen-Bonding-Induced Association of Poly(acrylic acid)- graft -poly(ethylene oxide) in Water journal, February 2010

Globule-to-Coil Transition of a Single Homopolymer Chain in Solution journal, May 1998

Kinetics of aggregation in micellar solutions of thermoresponsive triblock copolymers – influence of concentration, start and target temperatures journal, January 2013

Kinetics of Collapse Transition and Cluster Formation in a Thermoresponsive Micellar Solution of P(S-b-NIPAM-b-S) Induced by a Temperature Jump journal, January 2012

Mechanism of Microgel Formation via Cross-Linking of Polymers in Their Dilute Solutions: Mathematical Explanation with Computer Simulations journal, October 2001

On the hydrodynamic radius of fractal aggregates journal, November 1987

Light scattering studies on core–shell systems: determination of size parameters of sterically stabilized poly(methylmethacrylate) dispersions journal, April 2000

Structure formation of surfactants in concentrated sulphuric acid: a light scattering study journal, September 1995

Thermo-sensitive poly(N-vinylcaprolactam-co-acetoacetoxyethyl methacrylate) microgels: 1—synthesis and characterization journal, December 2003

Temperature-Controlled Assembly and Release from Polymer Vesicles of Poly(ethylene oxide)-block- poly(N-isopropylacrylamide) journal, November 2006

Reversibly crosslinked temperature-responsive nano-sized polymersomes: synthesis and triggered drug release journal, January 2009

Spectral interpretation of thermally irreversible recovery of poly(N-isopropylacrylamide-co-acrylic acid) hydrogel journal, January 2011

Homopolymer Self-Assembly into Stable Nanoparticles: Concerted Action of Hydrophobic Association and Hydrogen Bonding in Thermoresponsive Poly(alkylacrylic acid)s journal, February 2012

Volume phase transition in a nonionic gel journal, December 1984

Formation of an Intrapolymer Complex from Human Serum Albumin and Poly(ethylene glycol) journal, February 1999

Protein Separation via Polyelectrolyte Coacervation: Selectivity and Efficiency journal, June 1996

Charge Stoichiometry Inside Polyelectrolyte−Protein Complexes: A Direct SANS Measurement for the PSSNa−Lysozyme System journal, December 2006

Starch Fractions as Examples for Nonrandomly Branched Macromolecules. 4. Angular Dependence in Dynamic Light Scattering journal, November 1997

Formation of complexes in aqueous solutions of amphiphilic triblock polyelectrolytes of different topologies and an oppositely charged protein journal, January 2018

Emerging applications of stimuli-responsive polymer materials
journal, January 2010

Structure and design of polymeric surfactant-based drug delivery systems
journal, June 2001

Spherical polyelectrolyte brushes
journal, October 2007

Self-Cross-Linked Polymer Nanogels: A Versatile Nanoscopic Drug Delivery Platform
journal, December 2010

Thermoresponsive hydrogels in biomedical applications
journal, January 2008

Hydrogels in drug delivery: Progress and challenges
journal, April 2008

Microgels as Nanoreactors: Applications in Catalysis
book, January 2010

Reduction and temperature dual-responsive crosslinked polymersomes for targeted intracellular protein delivery
journal, January 2011

Morphological transitions in aggregates of thermosensitive poly(ethylene oxide)- b -poly( N -isopropylacrylamide) block copolymers prepared via RAFT polymerization: Morphological Transitions in PEO- b -PNIPAM
journal, July 2009

Living Radical Polymerization by the RAFT Process - A Second Update
journal, January 2009

Micellar and fractal aggregates formed by two triblock terpolymers with different arrangements of one charged, one neutral hydrophilic and one hydrophobic block
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Light Scattering by Fractal Aggregates: A Review
journal, January 2001

Dynamic light scattering study of internal motions of polymer coils in dilute solution
journal, December 1991

Asymptotic behavior and long-range interactions in aqueous solutions of poly(ethylene oxide)
journal, October 1991

Characterization of Poly(N-isopropylmethacrylamide) in Water
journal, December 1990

Structure of Micelles of Poly( n -butyl acrylate)- block -poly(acrylic acid) Diblock Copolymers in Aqueous Solution
journal, June 2007

Thermoresponsive transition of a PEO-b-PNIPAM copolymer: From hierarchical aggregates to well defined ellipsoidal vesicles
journal, November 2013

Thermoresponsive aggregation of PS–PNIPAM–PS triblock copolymer: A combined study of light scattering and small angle neutron scattering
journal, July 2014

Interchain Hydrogen-Bonding-Induced Association of Poly(acrylic acid)- graft -poly(ethylene oxide) in Water
journal, February 2010

Globule-to-Coil Transition of a Single Homopolymer Chain in Solution
journal, May 1998

Kinetics of aggregation in micellar solutions of thermoresponsive triblock copolymers – influence of concentration, start and target temperatures
journal, January 2013

Kinetics of Collapse Transition and Cluster Formation in a Thermoresponsive Micellar Solution of P(S-b-NIPAM-b-S) Induced by a Temperature Jump
journal, January 2012

Mechanism of Microgel Formation via Cross-Linking of Polymers in Their Dilute Solutions: Mathematical Explanation with Computer Simulations
journal, October 2001

On the hydrodynamic radius of fractal aggregates
journal, November 1987

Light scattering studies on core–shell systems: determination of size parameters of sterically stabilized poly(methylmethacrylate) dispersions
journal, April 2000

Structure formation of surfactants in concentrated sulphuric acid: a light scattering study
journal, September 1995

Thermo-sensitive poly(N-vinylcaprolactam-co-acetoacetoxyethyl methacrylate) microgels: 1—synthesis and characterization
journal, December 2003

Temperature-Controlled Assembly and Release from Polymer Vesicles of Poly(ethylene oxide)-block- poly(N-isopropylacrylamide)
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Reversibly crosslinked temperature-responsive nano-sized polymersomes: synthesis and triggered drug release
journal, January 2009

Spectral interpretation of thermally irreversible recovery of poly(N-isopropylacrylamide-co-acrylic acid) hydrogel
journal, January 2011

Homopolymer Self-Assembly into Stable Nanoparticles: Concerted Action of Hydrophobic Association and Hydrogen Bonding in Thermoresponsive Poly(alkylacrylic acid)s
journal, February 2012

Volume phase transition in a nonionic gel
journal, December 1984

Formation of an Intrapolymer Complex from Human Serum Albumin and Poly(ethylene glycol)
journal, February 1999

Protein Separation via Polyelectrolyte Coacervation: Selectivity and Efficiency
journal, June 1996

Charge Stoichiometry Inside Polyelectrolyte−Protein Complexes: A Direct SANS Measurement for the PSSNa−Lysozyme System
journal, December 2006

Starch Fractions as Examples for Nonrandomly Branched Macromolecules. 4. Angular Dependence in Dynamic Light Scattering
journal, November 1997

Formation of complexes in aqueous solutions of amphiphilic triblock polyelectrolytes of different topologies and an oppositely charged protein
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