Engineering the Structure and Rheological Properties of P407 Hydrogels via Reverse Poloxamer Addition

Joanna M. White; Ally Garza; James J. Griebler; Frank S. Bates; Michelle A. Calabrese

doi:10.1021/acs.langmuir.3c00088

Engineering the Structure and Rheological Properties of P407 Hydrogels via Reverse Poloxamer Addition

Joanna M. White
, Ally Garza
, James J. Griebler
, Frank S. Bates
, Michelle A. Calabrese

Research output: Contribution to journal › Article › peer-review

12 Scopus citations

Abstract

Aqueous solutions of poloxamer 407 (P407), a commercially available and nontoxic ABA triblock polymer (PEO-PPO-PEO), undergo a solution-to-gel transition with increasing temperature and are promising candidates for injectable therapeutics. The gel transition temperature, modulus, and structure are all dictated by polymer concentration, preventing independent tuning of these properties. Here, we show that addition of BAB reverse poloxamers (RPs) to P407-based solutions dramatically alters the gelation temperature, modulus, and morphology. Gelation temperature and RP localization within the hydrogel are dictated by RP solubility. Highly soluble RPs increase gelation temperature and incorporate primarily into the micelle corona regions. Alternatively, RPs with low aqueous solubility decrease gelation temperature and associate within the micelle core and core-corona interface. These differences in RP localization have significant implications for the hydrogel modulus and microstructure. The ability to tune gelation temperature, modulus, and structure through RP addition allows for the design of thermoresponsive materials with specific properties that are unobtainable with neat P407-based hydrogels.

Original language	English (US)
Pages (from-to)	5084-5094
Number of pages	11
Journal	Langmuir
Volume	39
Issue number	14
DOIs	https://doi.org/10.1021/acs.langmuir.3c00088
State	Published - Apr 11 2023

Bibliographical note

Funding Information:
Research reported in this publication was supported by the National Institute on Deafness and Other Communication Disorders of the National Institutes of Health under Award R21DC019184-01A1. Researchers contributing to this work were additionally supported by the National Science Foundation (NSF) Graduate Research Fellowship under Grant CON-75851, Project 00074041 (J.M. White), and through the Partnership for Research and Education in Materials (PREM) Program of the National Science Foundation under Award DMR-2122178 and the University of Minnesota MRSEC under Award Number DMR-2011401 (A. Garza). Any opinions, findings, and conclusions or recommendations expressed in this material are those of the author(s) and do not necessarily reflect the views of the National Science Foundation. This research used resources of the Advanced Photon Source, a U.S. Department of Energy (DOE) Office of Science User Facility, operated for the DOE Office of Science by Argonne National Laboratory under Contract DE-AC02-06CH11357. SAXS experiments were carried out at Sector 12-ID-B of the Advanced Photon Source. Lab-source SAXS experiments were carried out at the Characterization Facility, University of Minnesota, which receives partial support from the NSF through the MRSEC (Award Number DMR-2011401) and the NNCI (Award ECCS-2025124) programs. The authors thank the Anton Paar VIP program for the rheometer used in this work. NMR instruments used to collect data reported in this publication were purchased and maintained with support from the Office of the Vice President of Research, College of Science and Engineering, and the Department of Chemistry at the University of Minnesota.

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© 2023 American Chemical Society.

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@article{1aa37f93fd794ca68bd542be8c2f7b40,

title = "Engineering the Structure and Rheological Properties of P407 Hydrogels via Reverse Poloxamer Addition",

abstract = "Aqueous solutions of poloxamer 407 (P407), a commercially available and nontoxic ABA triblock polymer (PEO-PPO-PEO), undergo a solution-to-gel transition with increasing temperature and are promising candidates for injectable therapeutics. The gel transition temperature, modulus, and structure are all dictated by polymer concentration, preventing independent tuning of these properties. Here, we show that addition of BAB reverse poloxamers (RPs) to P407-based solutions dramatically alters the gelation temperature, modulus, and morphology. Gelation temperature and RP localization within the hydrogel are dictated by RP solubility. Highly soluble RPs increase gelation temperature and incorporate primarily into the micelle corona regions. Alternatively, RPs with low aqueous solubility decrease gelation temperature and associate within the micelle core and core-corona interface. These differences in RP localization have significant implications for the hydrogel modulus and microstructure. The ability to tune gelation temperature, modulus, and structure through RP addition allows for the design of thermoresponsive materials with specific properties that are unobtainable with neat P407-based hydrogels.",

author = "White, \{Joanna M.\} and Ally Garza and Griebler, \{James J.\} and Bates, \{Frank S.\} and Calabrese, \{Michelle A.\}",

note = "Funding Information: Research reported in this publication was supported by the National Institute on Deafness and Other Communication Disorders of the National Institutes of Health under Award R21DC019184-01A1. Researchers contributing to this work were additionally supported by the National Science Foundation (NSF) Graduate Research Fellowship under Grant CON-75851, Project 00074041 (J.M. White), and through the Partnership for Research and Education in Materials (PREM) Program of the National Science Foundation under Award DMR-2122178 and the University of Minnesota MRSEC under Award Number DMR-2011401 (A. Garza). Any opinions, findings, and conclusions or recommendations expressed in this material are those of the author(s) and do not necessarily reflect the views of the National Science Foundation. This research used resources of the Advanced Photon Source, a U.S. Department of Energy (DOE) Office of Science User Facility, operated for the DOE Office of Science by Argonne National Laboratory under Contract DE-AC02-06CH11357. SAXS experiments were carried out at Sector 12-ID-B of the Advanced Photon Source. Lab-source SAXS experiments were carried out at the Characterization Facility, University of Minnesota, which receives partial support from the NSF through the MRSEC (Award Number DMR-2011401) and the NNCI (Award ECCS-2025124) programs. The authors thank the Anton Paar VIP program for the rheometer used in this work. NMR instruments used to collect data reported in this publication were purchased and maintained with support from the Office of the Vice President of Research, College of Science and Engineering, and the Department of Chemistry at the University of Minnesota. Publisher Copyright: {\textcopyright} 2023 American Chemical Society.",

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N2 - Aqueous solutions of poloxamer 407 (P407), a commercially available and nontoxic ABA triblock polymer (PEO-PPO-PEO), undergo a solution-to-gel transition with increasing temperature and are promising candidates for injectable therapeutics. The gel transition temperature, modulus, and structure are all dictated by polymer concentration, preventing independent tuning of these properties. Here, we show that addition of BAB reverse poloxamers (RPs) to P407-based solutions dramatically alters the gelation temperature, modulus, and morphology. Gelation temperature and RP localization within the hydrogel are dictated by RP solubility. Highly soluble RPs increase gelation temperature and incorporate primarily into the micelle corona regions. Alternatively, RPs with low aqueous solubility decrease gelation temperature and associate within the micelle core and core-corona interface. These differences in RP localization have significant implications for the hydrogel modulus and microstructure. The ability to tune gelation temperature, modulus, and structure through RP addition allows for the design of thermoresponsive materials with specific properties that are unobtainable with neat P407-based hydrogels.

AB - Aqueous solutions of poloxamer 407 (P407), a commercially available and nontoxic ABA triblock polymer (PEO-PPO-PEO), undergo a solution-to-gel transition with increasing temperature and are promising candidates for injectable therapeutics. The gel transition temperature, modulus, and structure are all dictated by polymer concentration, preventing independent tuning of these properties. Here, we show that addition of BAB reverse poloxamers (RPs) to P407-based solutions dramatically alters the gelation temperature, modulus, and morphology. Gelation temperature and RP localization within the hydrogel are dictated by RP solubility. Highly soluble RPs increase gelation temperature and incorporate primarily into the micelle corona regions. Alternatively, RPs with low aqueous solubility decrease gelation temperature and associate within the micelle core and core-corona interface. These differences in RP localization have significant implications for the hydrogel modulus and microstructure. The ability to tune gelation temperature, modulus, and structure through RP addition allows for the design of thermoresponsive materials with specific properties that are unobtainable with neat P407-based hydrogels.

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Engineering the Structure and Rheological Properties of P407 Hydrogels via Reverse Poloxamer Addition

Abstract

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Partnership for Research and Education in Materials

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REU Site: Science and Engineering in Nanomaterials

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Engineering the Structure and Rheological Properties of P407 Hydrogels via Reverse Poloxamer Addition

Abstract

Bibliographical note

MRSEC Support

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Projects

Partnership for Research and Education in Materials

University of Minnesota Materials Research Science and Engineering Center (DMR-2011401)

REU Site: Science and Engineering in Nanomaterials

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