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Title: Poly(vinyl alcohol) Hydrogels with Broad-Range Tunable Mechanical Properties via the Hofmeister Effect

Abstract

Hydrogels, exhibiting wide applications in soft robotics, tissue engineering, implantable electronics, etc., often require sophisticately tailoring of the hydrogel mechanical properties to meet specific demands. For examples, soft robotics necessitates tough hydrogels; stem cell culturing demands various tissue-matching modulus; and neuron probes desire dynamically tunable modulus. Herein, a strategy to broadly alter the mechanical properties of hydrogels reversibly via tuning the aggregation states of the polymer chains by ions based on the Hofmeister effect is reported. An ultratough poly(vinyl alcohol) (PVA) hydrogel as an exemplary material (toughness 150 ± 20 MJ m-3), which surpasses synthetic polymers like poly(dimethylsiloxane), synthetic rubber, and natural spider silk is fabricated. With various ions, the hydrogel's various mechanical properties are continuously and reversibly in situ modulated over a large window: tensile strength from 50 ± 9 kPa to 15 ± 1 MPa, toughness from 0.0167 ± 0.003 to 150 ± 20 MJ m-3, elongation from 300 ± 100% to 2100 ± 300%, and modulus from 24 ± 2 to 2500 ± 140 kPa. Importantly, the ions serve as gelation triggers and property modulators only, not necessarily required to remain in the gel, maintaining the high biocompatibility of PVA without excess ions. Overall, this strategy, enablingmore » high mechanical performance and broad dynamic tunability, presents a universal platform for broad applications from biomedicine to wearable electronics.« less

Authors:
ORCiD logo [1];  [2];  [2];  [2];  [2];  [2];  [2];  [2];  [2];  [1];  [3];  [3];  [4]; ORCiD logo [2]
  1. Univ. of California, Los Angeles, CA (United States); Shanghai Jiao Tong Univ. (China). State Key Lab. of Metal Matrix Composites
  2. Univ. of California, Los Angeles, CA (United States)
  3. Argonne National Lab. (ANL), Argonne, IL (United States)
  4. Shanghai Jiao Tong Univ. (China). State Key Lab. of Metal Matrix Composites
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
National Science Foundation (NSF); US Air Force Office of Scientific Research (AFOSR); US Office of Naval Research (ONR); USDOE Office of Science (SC)
OSTI Identifier:
1774628
Grant/Contract Number:  
AC02-06CH11357; 1724526; FA9550-17-1-0311; FA9550-18-1-0449; FA9550-20-1-0344; N000141712117; N00014-18-1-2314
Resource Type:
Accepted Manuscript
Journal Name:
Advanced Materials
Additional Journal Information:
Journal Volume: 33; Journal Issue: 11; Journal ID: ISSN 0935-9648
Publisher:
Wiley
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; Hofmeister effect; ions; poly (vinyl alcohol); tough hydrogel; tunable mechanical properties

Citation Formats

Wu, Shuwang, Hua, Mutian, Alsaid, Yousif, Du, Yingjie, Ma, Yanfei, Zhao, Yusen, Lo, Chiao‐Yueh, Wang, Canran, Wu, Dong, Yao, Bowen, Strzalka, Joseph, Zhou, Hua, Zhu, Xinyuan, and He, Ximin. Poly(vinyl alcohol) Hydrogels with Broad-Range Tunable Mechanical Properties via the Hofmeister Effect. United States: N. p., 2021. Web. doi:10.1002/adma.202007829.
Wu, Shuwang, Hua, Mutian, Alsaid, Yousif, Du, Yingjie, Ma, Yanfei, Zhao, Yusen, Lo, Chiao‐Yueh, Wang, Canran, Wu, Dong, Yao, Bowen, Strzalka, Joseph, Zhou, Hua, Zhu, Xinyuan, & He, Ximin. Poly(vinyl alcohol) Hydrogels with Broad-Range Tunable Mechanical Properties via the Hofmeister Effect. United States. https://doi.org/10.1002/adma.202007829
Wu, Shuwang, Hua, Mutian, Alsaid, Yousif, Du, Yingjie, Ma, Yanfei, Zhao, Yusen, Lo, Chiao‐Yueh, Wang, Canran, Wu, Dong, Yao, Bowen, Strzalka, Joseph, Zhou, Hua, Zhu, Xinyuan, and He, Ximin. Mon . "Poly(vinyl alcohol) Hydrogels with Broad-Range Tunable Mechanical Properties via the Hofmeister Effect". United States. https://doi.org/10.1002/adma.202007829. https://www.osti.gov/servlets/purl/1774628.
@article{osti_1774628,
title = {Poly(vinyl alcohol) Hydrogels with Broad-Range Tunable Mechanical Properties via the Hofmeister Effect},
author = {Wu, Shuwang and Hua, Mutian and Alsaid, Yousif and Du, Yingjie and Ma, Yanfei and Zhao, Yusen and Lo, Chiao‐Yueh and Wang, Canran and Wu, Dong and Yao, Bowen and Strzalka, Joseph and Zhou, Hua and Zhu, Xinyuan and He, Ximin},
abstractNote = {Hydrogels, exhibiting wide applications in soft robotics, tissue engineering, implantable electronics, etc., often require sophisticately tailoring of the hydrogel mechanical properties to meet specific demands. For examples, soft robotics necessitates tough hydrogels; stem cell culturing demands various tissue-matching modulus; and neuron probes desire dynamically tunable modulus. Herein, a strategy to broadly alter the mechanical properties of hydrogels reversibly via tuning the aggregation states of the polymer chains by ions based on the Hofmeister effect is reported. An ultratough poly(vinyl alcohol) (PVA) hydrogel as an exemplary material (toughness 150 ± 20 MJ m-3), which surpasses synthetic polymers like poly(dimethylsiloxane), synthetic rubber, and natural spider silk is fabricated. With various ions, the hydrogel's various mechanical properties are continuously and reversibly in situ modulated over a large window: tensile strength from 50 ± 9 kPa to 15 ± 1 MPa, toughness from 0.0167 ± 0.003 to 150 ± 20 MJ m-3, elongation from 300 ± 100% to 2100 ± 300%, and modulus from 24 ± 2 to 2500 ± 140 kPa. Importantly, the ions serve as gelation triggers and property modulators only, not necessarily required to remain in the gel, maintaining the high biocompatibility of PVA without excess ions. Overall, this strategy, enabling high mechanical performance and broad dynamic tunability, presents a universal platform for broad applications from biomedicine to wearable electronics.},
doi = {10.1002/adma.202007829},
journal = {Advanced Materials},
number = 11,
volume = 33,
place = {United States},
year = {Mon Feb 08 00:00:00 EST 2021},
month = {Mon Feb 08 00:00:00 EST 2021}
}

Works referenced in this record:

Highly stretchable and tough hydrogels
journal, September 2012

  • Sun, Jeong-Yun; Zhao, Xuanhe; Illeperuma, Widusha R. K.
  • Nature, Vol. 489, Issue 7414
  • DOI: 10.1038/nature11409

A Universal Soaking Strategy to Convert Composite Hydrogels into Extremely Tough and Rapidly Recoverable Double-Network Hydrogels
journal, June 2016


Hydrogels with tunable stress relaxation regulate stem cell fate and activity
journal, November 2015

  • Chaudhuri, Ovijit; Gu, Luo; Klumpers, Darinka
  • Nature Materials, Vol. 15, Issue 3
  • DOI: 10.1038/nmat4489

Hofmeister Salt Effects on Surface Tension Arise from Partitioning of Anions and Cations between Bulk Water and the Air−Water Interface
journal, May 2007

  • Pegram, Laurel M.; Record, M. Thomas
  • The Journal of Physical Chemistry B, Vol. 111, Issue 19
  • DOI: 10.1021/jp070245z

Spontaneously Regenerative Tough Hydrogels
journal, July 2019


Effects of substrate stiffness and cell-cell contact on mesenchymal stem cell differentiation
journal, August 2016


Naturally biomimicked smart shape memory hydrogels for biomedical functions
journal, January 2020


Interactions between macromolecules and ions: the Hofmeister series
journal, December 2006


Designing hydrogels for controlled drug delivery
journal, October 2016


Tuning Hydrogel Mechanics Using the Hofmeister Effect
journal, September 2015

  • Jaspers, Maarten; Rowan, Alan E.; Kouwer, Paul H. J.
  • Advanced Functional Materials, Vol. 25, Issue 41
  • DOI: 10.1002/adfm.201502241

Hydraulic hydrogel actuators and robots optically and sonically camouflaged in water
journal, February 2017

  • Yuk, Hyunwoo; Lin, Shaoting; Ma, Chu
  • Nature Communications, Vol. 8, Issue 1
  • DOI: 10.1038/ncomms14230

The influence of substrate stiffness gradients on primary human dermal fibroblasts
journal, July 2013


Stimuli-Responsive Polymer Nanocomposites Inspired by the Sea Cucumber Dermis
journal, March 2008

  • Capadona, J. R.; Shanmuganathan, K.; Tyler, D. J.
  • Science, Vol. 319, Issue 5868, p. 1370-1374
  • DOI: 10.1126/science.1153307

Ion-specific swelling of hydrophilic polymer gels
journal, June 2001


Specific Ion Effects on the Water Solubility of Macromolecules:  PNIPAM and the Hofmeister Series
journal, October 2005

  • Zhang, Yanjie; Furyk, Steven; Bergbreiter, David E.
  • Journal of the American Chemical Society, Vol. 127, Issue 41
  • DOI: 10.1021/ja0546424

Soft and elastic hydrogel-based microelectronics for localized low-voltage neuromodulation
journal, January 2019


Beyond Hofmeister
journal, March 2014

  • Jungwirth, Pavel; Cremer, Paul S.
  • Nature Chemistry, Vol. 6, Issue 4
  • DOI: 10.1038/nchem.1899

Stem cell migration and mechanotransduction on linear stiffness gradient hydrogels
journal, May 2017

  • Hadden, William J.; Young, Jennifer L.; Holle, Andrew W.
  • Proceedings of the National Academy of Sciences, Vol. 114, Issue 22
  • DOI: 10.1073/pnas.1618239114

Molecularly Engineered Dual-Crosslinked Hydrogel with Ultrahigh Mechanical Strength, Toughness, and Good Self-Recovery
journal, February 2015


Hydrogels for Engineering of Perfusable Vascular Networks
journal, July 2015

  • Liu, Juan; Zheng, Huaiyuan; Poh, Patrina
  • International Journal of Molecular Sciences, Vol. 16, Issue 7
  • DOI: 10.3390/ijms160715997

Kinetic behaviour of the cells touching substrate: the interfacial stiffness guides cell spreading
journal, January 2014

  • Li, Jianjun; Han, Dong; Zhao, Ya-Pu
  • Scientific Reports, Vol. 4, Issue 1
  • DOI: 10.1038/srep03910

Dual-Stimuli-Responsive Polymer Composite with Ultrawide Tunable Stiffness Range Triggered by Water and Temperature
journal, April 2020

  • Qiu, Yu; Askounis, Erin; Guan, Fangyi
  • ACS Applied Polymer Materials, Vol. 2, Issue 5
  • DOI: 10.1021/acsapm.0c00181

Novel PVA-based polymers showing an anti-Hofmeister Series property
journal, July 2009


Hofmeister Phenomena: An Update on Ion Specificity in Biology
journal, January 2012

  • Lo Nostro, Pierandrea; Ninham, Barry W.
  • Chemical Reviews, Vol. 112, Issue 4
  • DOI: 10.1021/cr200271j

Mussel-Inspired Adhesive and Tough Hydrogel Based on Nanoclay Confined Dopamine Polymerization
journal, February 2017


Anion Complexation and The Hofmeister Effect
journal, September 2014

  • Carnegie, Ryan S.; Gibb, Corinne L. D.; Gibb, Bruce C.
  • Angewandte Chemie International Edition, Vol. 53, Issue 43
  • DOI: 10.1002/anie.201405796

PVA-based hydrogels for tissue engineering: A review
journal, June 2016

  • Kumar, Anuj; Han, Sung Soo
  • International Journal of Polymeric Materials and Polymeric Biomaterials, Vol. 66, Issue 4
  • DOI: 10.1080/00914037.2016.1190930

Ion-specific ice recrystallization provides a facile approach for the fabrication of porous materials
journal, May 2017

  • Wu, Shuwang; Zhu, Chongqin; He, Zhiyuan
  • Nature Communications, Vol. 8, Issue 1
  • DOI: 10.1038/ncomms15154

Specific ion effects directed noble metal aerogels: Versatile manipulation for electrocatalysis and beyond
journal, May 2019


Muscle-like fatigue-resistant hydrogels by mechanical training
journal, May 2019

  • Lin, Shaoting; Liu, Ji; Liu, Xinyue
  • Proceedings of the National Academy of Sciences, Vol. 116, Issue 21
  • DOI: 10.1073/pnas.1903019116

Freezing Molecular Orientation under Stretch for High Mechanical Strength but Anisotropic Hydrogels
journal, July 2016


Hydrogel Paint
journal, August 2019


A Facile Method to Fabricate Anisotropic Hydrogels with Perfectly Aligned Hierarchical Fibrous Structures
journal, January 2018

  • Mredha, Md. Tariful Islam; Guo, Yun Zhou; Nonoyama, Takayuki
  • Advanced Materials, Vol. 30, Issue 9
  • DOI: 10.1002/adma.201704937

Fabrication of Bioinspired Hydrogels: Challenges and Opportunities
journal, April 2020


The effects of hyaluronic acid hydrogels with tunable mechanical properties on neural progenitor cell differentiation
journal, May 2010


Weak Hydrogen Bonding Enables Hard, Strong, Tough, and Elastic Hydrogels
journal, October 2015

  • Hu, Xiaobo; Vatankhah-Varnoosfaderani, Mohammad; Zhou, Jing
  • Advanced Materials, Vol. 27, Issue 43
  • DOI: 10.1002/adma.201503724

Erratum to: Increased microenvironment stiffness in damaged myofibers promotes myogenic progenitor cell proliferation
journal, September 2015


Tuning the mechanical properties of bioreducible multilayer films for improved cell adhesion and transfection activity
journal, September 2010


An Intrinsically Stretchable and Compressible Supercapacitor Containing a Polyacrylamide Hydrogel Electrolyte
journal, June 2017

  • Huang, Yan; Zhong, Ming; Shi, Fukuan
  • Angewandte Chemie International Edition, Vol. 56, Issue 31
  • DOI: 10.1002/anie.201705212

Hofmeister Effect-Assisted One Step Fabrication of Ductile and Strong Gelatin Hydrogels
journal, December 2017

  • He, Qingyan; Huang, Yan; Wang, Shaoyun
  • Advanced Functional Materials, Vol. 28, Issue 5
  • DOI: 10.1002/adfm.201705069

Tissue Stiffness Dictates Development, Homeostasis, and Disease Progression
journal, January 2015


Tough bonding of hydrogels to diverse non-porous surfaces
journal, November 2015

  • Yuk, Hyunwoo; Zhang, Teng; Lin, Shaoting
  • Nature Materials, Vol. 15, Issue 2
  • DOI: 10.1038/nmat4463

Hydrogels for Tissue Engineering
journal, July 2001

  • Lee, Kuen Yong; Mooney, David J.
  • Chemical Reviews, Vol. 101, Issue 7
  • DOI: 10.1021/cr000108x

Anti-fatigue-fracture hydrogels
journal, January 2019