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Metals & Polymers In The Mix: Fine-tuning The Mechanical Properties & Color Of Self-healing Mussel-inspired Hydrogels.

M. Krogsgaard, M. R. Hansen, Henrik Birkedal
Published 2014 · Materials Science, Medicine

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Reversible sacrificial bonds play a crucial role in various biological materials where they serve as load-bearing bonds, facilitating extensibility and/or impart self-healing properties to the biological materials. Recently, the coordination bonds found in blue mussel byssal threads have been mimicked in the design of self-healing hydrogels. Herein we show how the mechanical moduli of mussel-inspired hydrogels based on DOPA-polyallylamine (DOPA-PAA) can be straight-forwardly adjusted by systematically varying the coordinating metal from AlIII, GaIII to InIII. These gels are transparent and only slightly tanned opposite to the black hydrogels obtained using FeIII. Additionally, dark FeIII:DOPA-chitosan gels were synthesized and showed remarkably high storage modulus. The strongest hydrogels were formed around pH 8, which is closer to physiological pH than what was observed in the FeIII:DOPA-PAA system (pHmax∼ 9.5). This finding supports the hypothesis that the maximum in the storage modulus distribution can be adjusted to match a given application by selecting the cationic polymer based on its pKa value.
This paper references
10.1039/C3SM51824H
Versatile tuning of supramolecular hydrogels through metal complexation of oxidation-resistant catechol-inspired ligands.
M. Menyo (2013)
Chem
N. Holten-Andersen (2012)
10.1021/MA301791N
Mussel-inspired histidine-based transient network metal coordination hydrogels.
Dominic E Fullenkamp (2013)
10.1038/NMAT1956
Protective coatings on extensible biofibres.
N. Holten-Andersen (2007)
10.1016/S0378-5173(98)00378-0
Potential of low molecular mass chitosan as a DNA delivery system: biocompatibility, body distribution and ability to complex and protect DNA.
S. Richardson (1999)
10.1021/MA300962D
Ambivalent Adhesives: Combining Biomimetic Cross-Linking With Antiadhesive Oligo(ethylene glycol).
Cristina R. Matos-perez (2012)
10.1017/CBO9781139207249.009
I and J
William M. Marsden (2012)
10.1021/jp408864s
Temperature-regulated fluorescence and association of an oligo(ethyleneglycol)methacrylate-based copolymer with a conjugated polyelectrolyte--the effect of solution ionic strength.
Sahika Inal (2013)
10.1039/C3TB21374A
Metal-coordination: Using one of nature's tricks to control soft material mechanics.
Niels Holten-Andersen (2014)
10.1039/9781847550682
d- and f-Block Chemistry
C. Jones (2002)
and X
J. H. Wait (2001)
10.1021/BI002718X
Polyphosphoprotein from the adhesive pads of Mytilus edulis.
J. Waite (2001)
10.1002/(SICI)1099-0534(1997)9:6<433::AID-CMR5>3.0.CO;2-#
Multidimensional solid-state NMR and polymers
K. W. Zilm (1997)
10.1021/bm8006659
Ragworm jaw-inspired metal ion cross-linking for improved mechanical properties of polymer blends.
A. Srivastava (2008)
10.1073/pnas.1007416107
Strong reversible Fe3+-mediated bridging between dopa-containing protein films in water
Hongbo Zeng (2010)
10.1016/S0065-2806(10)38003-9
Diverse Strategies of Protein Sclerotization in Marine Invertebrates: Structure–Property Relationships in Natural Biomaterials
D. J. Rubin (2010)
10.1021/bm4017308
Mussel-mimetic protein-based adhesive hydrogel.
B. J. Kim (2014)
10.1021/IC960514S
Ferric Ion Complexes of a DOPA-Containing Adhesive Protein from Mytilus edulis
S. W. Taylor (1996)
Comp
J. H. Waite (1990)
10.1002/anie.201108629
Bioinspired underwater bonding and debonding on demand.
Zahid Shafiq (2012)
10.1039/c4cc05293e
Gels and threads: mussel-inspired one-pot route to advanced responsive materials.
M. Krogsgaard (2014)
10.1073/pnas.1632658100
Zinc and mechanical prowess in the jaws of Nereis, a marine worm
H. Lichtenegger (2003)
10.1002/ADFM.201201106
Functional nanogels as platforms for imparting antibacterial, antibiofilm, and antiadhesion activities to stainless steel
E. Faure (2012)
and P
D. E. Fullenkamp (2013)
Chem
H. G. Jang (1991)
Cur
T. J. Deming (1999)
10.1002/adma.201202343
Catechol-based biomimetic functional materials.
J. Sedó (2013)
10.1021/BM025546N
Synthesis and gelation of DOPA-modified poly(ethylene glycol) hydrogels.
B. P. Lee (2002)
10.1126/science.1181044
Iron-Clad Fibers: A Metal-Based Biological Strategy for Hard Flexible Coatings
Matthew J. Harrington (2010)
10.1016/S0939-6411(03)00161-9
Structure and interactions in covalently and ionically crosslinked chitosan hydrogels for biomedical applications.
J. Berger (2004)
10.1016/S0142-9612(96)00167-6
In vitro and in vivo degradation of films of chitin and its deacetylated derivatives.
K. Tomihata (1997)
10.1021/MA961766F
Biodegradation of Cross-Linked Chitosan Gels by a Microorganism
H. Yamamoto (1997)
Inorg
S. W. Taylor (1996)
10.1039/C4RA03178D
pH-dependent cross-linking of catechols through oxidation via Fe3+ and potential implications for mussel adhesion.
Dominic E Fullenkamp (2014)
10.1016/S0939-6411(03)00160-7
Structure and interactions in chitosan hydrogels formed by complexation or aggregation for biomedical applications.
J. Berger (2004)
Annu
B. P. Lee (2011)
10.1021/bm301844u
Self-healing mussel-inspired multi-pH-responsive hydrogels.
M. Krogsgaard (2013)
10.1039/C3PY00788J
Rapid self-healing and triple stimuli responsiveness of a supramolecular polymer gel based on boron–catechol interactions in a novel water-soluble mussel-inspired copolymer
Mohammad Vatankhah-Varnoosfaderani (2014)
10.1038/nature05968
A reversible wet/dry adhesive inspired by mussels and geckos
H. Lee (2007)
10.1126/SCIENCE.1147241
Mussel-Inspired Surface Chemistry for Multifunctional Coatings
H. Lee (2007)
10.1038/nchembio.630
Mussel protein adhesion depends on thiol-mediated redox modulation
J. Yu (2011)
10.1021/la8027012
Metals and the integrity of a biological coating: the cuticle of mussel byssus.
N. Holten-Andersen (2009)
10.1016/S1367-5931(99)80018-0
Mussel byssus and biomolecular materials.
T. Deming (1999)
Nature Chem
J. Yu (2012)
10.1021/JA00024A028
A Highly Reactive Functional Model for the Catechol Dioxygenases. Structure and Properties of [Fe(TPA)DBC]BPh4
H. Jang (1991)
10.1021/nn502240r
Seamless Metallic Coating and Surface Adhesion of Self-Assembled Bioinspired Nanostructures Based on Di-(3,4-dihydroxy-l-phenylalanine) Peptide Motif
Galit Fichman (2014)
10.1021/bm201261d
Enzymatically Degradable Mussel-Inspired Adhesive Hydrogel
C. Brubaker (2011)
10.1021/ja303369p
Polymer composition and substrate influences on the adhesive bonding of a biomimetic, cross-linking polymer.
Cristina R. Matos-perez (2012)
10.1002/btpr.1691
A biomimetic chitosan composite with improved mechanical properties in wet conditions
D. Oh (2013)
10.1073/pnas.0605552103
Single-molecule mechanics of mussel adhesion
H. Lee (2006)
10.1002/adma.201203362
Antibacterial strategies from the sea: polymer-bound cl-catechols for prevention of biofilm formation.
Luis García-Fernández (2013)
Int
S. W. Richardson (1999)
10.1002/ANIE.200352759
Metal-mediated cross-linking in the generation of a marine-mussel adhesive.
M. J. Sever (2004)
10.1016/J.PMATSCI.2007.05.002
Biological materials: Structure and mechanical properties
M. Meyers (2008)
10.1021/bm200464x
Catechol-functionalized chitosan/pluronic hydrogels for tissue adhesives and hemostatic materials.
J. H. Ryu (2011)
10.1073/pnas.1015862108
pH-induced metal-ligand cross-links inspired by mussel yield self-healing polymer networks with near-covalent elastic moduli
Niels Holten-Andersen (2011)
10.1021/CM302301E
Mussel-Inspired Thiol–Ene Polymer Networks: Influencing Network Properties and Adhesion with Catechol Functionality
B. Sparks (2012)
10.1146/ANNUREV-MATSCI-062910-100429
Mussel-Inspired Adhesives and Coatings.
B. P. Lee (2011)
10.1126/science.1237265
One-Step Assembly of Coordination Complexes for Versatile Film and Particle Engineering
Hirotaka Ejima (2013)
10.1002/cbic.200600160
Halogenated Veneers: Protein Cross‐Linking and Halogenation in the Jaws of Nereis, a Marine Polychaete Worm
Henrik Birkedal  (2006)
10.1021/jp210043w
pH- and voltage-responsive chitosan hydrogel through covalent cross-linking with catechol.
Yongchao Zhang (2012)



This paper is referenced by
10.1021/acsami.6b08220
Self-Healing Polymer Dielectric for a High Capacitance Gate Insulator.
Jieun Ko (2016)
10.1021/acsami.7b09614
High-Strength, Tough, and Self-Healing Nanocomposite Physical Hydrogels Based on the Synergistic Effects of Dynamic Hydrogen Bond and Dual Coordination Bonds.
Changyou Shao (2017)
10.1002/adma.201805091
Iron Gall Ink Revisited: In Situ Oxidation of Fe(II)-Tannin Complex for Fluidic-Interface Engineering.
Hojae Lee (2018)
10.1039/C8TB02854K
Electrochemical-Mediated Gelation Of Catechol-Bearing Hydrogels Based On Multimodal Crosslinking.
Chenchen Mou (2019)
10.1039/C7RA09621F
Facile one-pot synthesis and self-healing properties of tetrazole-based metallopolymers in the presence of iron salts
W. Wang (2017)
10.1016/J.SURFCOAT.2015.12.054
Enhancement of high temperature oxidation resistance and spallation resistance of SiC-self-healing thermal barrier coatings
Taoyuan Ouyang (2016)
10.1016/J.EURPOLYMJ.2017.05.020
Reversible interactions in self-healing and shape memory hydrogels
B. Gyarmati (2017)
10.1002/adma.201601613
Self-Healing Hydrogels.
D. Taylor (2016)
10.1021/acs.biomac.7b01249
Mussel-Inspired Self-Healing Double-Cross-Linked Hydrogels by Controlled Combination of Metal Coordination and Covalent Cross-Linking.
A. Andersen (2018)
10.1002/chem.201503380
Mussel-Inspired Materials: Self-Healing through Coordination Chemistry.
M. Krogsgaard (2016)
10.1021/acs.biomac.7b00321
Enzyme-Regulated Fast Self-Healing of a Pillararene-Based Hydrogel.
Xin Zhang (2017)
10.1039/C6TB03052A
Weak Bond-Based Injectable and Stimuli Responsive Hydrogels for Biomedical Applications.
Xiaochu Ding (2017)
10.1002/pola.28368
Recent approaches in designing bioadhesive materials inspired by mussel adhesive protein
Pegah Kord Forooshani (2017)
10.1016/j.ijbiomac.2018.04.088
Glycogen-based self-healing hydrogels with ultra-stretchable, flexible, and enhanced mechanical properties via sacrificial bond interactions.
I. Hussain (2018)
10.1021/acsami.8b13589
Spray Assembly of Metal-Phenolic Networks: Formation, Growth, and Applications.
Qi-Zhi Zhong (2018)
10.1021/ACSMACROLETT.5B00664
Rate-Dependent Stiffness and Recovery in Interpenetrating Network Hydrogels through Sacrificial Metal Coordination Bonds.
M. Menyo (2015)
10.1002/ADFM.201804416
Salt‐Mediated Polyampholyte Hydrogels with High Mechanical Strength, Excellent Self‐Healing Property, and Satisfactory Electrical Conductivity
Tangjie Long (2018)
10.1016/J.ELECTACTA.2019.06.180
Electrochemical deposition of bio-inspired laccase-polydopamine films for phenolic sensors
L. Almeida (2019)
10.3390/biomimetics4010020
Healing through Histidine: Bioinspired Pathways to Self-Healing Polymers via Imidazole–Metal Coordination
Stefan Zechel (2019)
10.1039/c9nr09780e
Recent progress in synthesis and application of mussel-inspired adhesives.
Q. Guo (2020)
10.1016/j.jconrel.2019.11.006
Chitosan oral patches inspired by mussel adhesion.
J. H. Ryu (2019)
10.1021/acsomega.7b01067
Tannic Acid-Based Multifunctional Hydrogels with Facile Adjustable Adhesion and Cohesion Contributed by Polyphenol Supramolecular Chemistry
Hailong Fan (2017)
10.1007/s13233-019-7032-5
Synthesis and Properties of Self-healing Metallopolymers with 5-Vinyltetrazole Units and Zn(II)
Mifa Chen (2018)
10.1002/ADMI.201500298
Polyphenol/FeIII Complex Coated Membranes Having Multifunctional Properties Prepared by a One‐Step Fast Assembly
H. Kim (2015)
10.1016/j.actbio.2015.08.043
Bio-inspired adhesive catechol-conjugated chitosan for biomedical applications: A mini review.
J. H. Ryu (2015)
10.1021/ACS.CHEMMATER.6B03676
Switch of Surface Adhesion to Cohesion by Dopa-Fe3+ Complexation, in Response to Microenvironment at the Mussel Plaque/Substrate Interface
Byeongseon Yang (2016)
10.1098/rsif.2015.0466
Mechanical homeostasis of a DOPA-enriched biological coating from mussels in response to metal variation
C. Schmitt (2015)
10.1007/978-981-10-6077-9_16
Hydrogels from Catechol-Conjugated Polymeric Materials
S. Moulay (2018)
10.1002/adma.201700759
Bioinspired Ultratough Hydrogel with Fast Recovery, Self-Healing, Injectability and Cytocompatibility.
S. Azevedo (2017)
10.1002/adma.201704640
Bioinspired Underwater Adhesives by Using the Supramolecular Toolbox.
Anton H. Hofman (2018)
10.1007/s10853-020-05252-8
An autonomous self-healing hydrogel with high polydopamine content for improved tensile strength
Jin-xin Huang (2020)
10.1073/pnas.1919712117
Compartmentalized processing of catechols during mussel byssus fabrication determines the destiny of DOPA
Tobias Priemel (2020)
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