J. Mater. Sci. Technol. ›› 2021, Vol. 63: 35-53.DOI: 10.1016/j.jmst.2020.02.052
• Research Article • Previous Articles Next Articles
Gopinathan Janarthanana,b, Insup Noha,b,*()
Received:
2019-11-28
Revised:
2020-01-29
Accepted:
2020-02-04
Published:
2021-02-10
Online:
2021-02-15
Contact:
Insup Noh
About author:
*Department of Chemical and Biomolecular Engineering, Seoul National University of Science and Technology, Seoul, 01811, Republic of Korea.E-mail address: insup@seoultech.ac.kr (I. Noh).Gopinathan Janarthanan, Insup Noh. Recent trends in metal ion based hydrogel biomaterials for tissue engineering and other biomedical applications[J]. J. Mater. Sci. Technol., 2021, 63: 35-53.
S.No. | Polymers | Metal Ions | Mechanism | In vitro studies | In vivo studies | Application | Ref |
---|---|---|---|---|---|---|---|
1 | Thiolate/Disulfide exchange | Au+, Ag+ | Thiols and thilolates protection from aerial oxidation with the help of Au and Ag ions by forming Au-S/di-sulphide (SS) (or Ag-S/SS) exchange | Human dermal fibroblasts (HDFs) | No | Potential use as a medical device | [ |
2 | Alginate/CMC | Fe3+ | High electrostatic attractions between carboxylic groups of alginate/CMC and the Fe3+ ions | No | No | Drug delivery | [ |
3 | Plant-origin poly(uronic acid) (PUA) | Fe3+ | Fe3+-polyuronate metal coordination complexes formed from photochemical reaction with visible light irradiation | No | No | Drug delivery | [ |
4 | Poly(dimethyl diallyl ammonium chloride)/Tannic acid (PDDA/TA) | Fe3+ | Multiple pyrogallol TA interacts with PDDA chains through ionic bonds and polymer chains are cross-linked to form networks with the Fe3+ ion coordination | No | No | Other (Adhesion and Cohesion) | [ |
5 | Polygalacturonate | Fe2+ | The galacto-uronate units are cross-linked by interacting with Fe2+ ions | No | No | Biocompatible materials | [ |
6 | Poly(acrylamide-co-acrylic acid) | Fe3+ | The acrylic units are covalently cross-linked and the carboxylate groups and Fe3+ ions form the ionic crosslinking | L929 | No | Biocompatible materials | [ |
7 | Poly(ethylene glycol)- 2,6‐pyridinedicarbonyl (H2pdca)/Poly(acrylic acid) (PAA) | Fe3+ | PEG‐H2pdca form the initial network with metal-ligand interactions. Second network from AA polymerization and cross‐linking through Fe3+ ions | No | No | Electronic skin | [ |
8 | Poly(N-acryloyl glycinamide) PNAGA /Carboxymethyl cellulose (CMC) | Fe3+ | PNAGA cross-linked via hydrogen bonds and CMC cross-linked via Fe3+ ion metal coordination forming dual networks | MTT test | No | Soft T.E | [ |
9 | Polyacrylamide (PAM)/Sodium alginate (SA) | Ag+, Ca2+, Fe3+, Cu2+, Ni2+, Co2+ | For dual network formation PAM/SA was polymerized first and then followed by metal-ion coordination by immersing it in the metal ion solutions and then recovery solutions were used to check the shape recovery. | No | No | Biomedical | [ |
10 | Poly(N,N’-dimethylacrylamide-co-glycidyl methacrylate) (PDMA) | Eu3+ | PDMA consisting of hydrophilic iminodiacetate interacts with lanthanide metal ions dynamically and under stimuli (pH & heating) associate and disassociate | No | No | Biomedical (Biological sensors) | [ |
11 | Xanthan gum | Fe3+ | Coordination bond formation between the Fe3+ ions and the carboxylate groups of xanthan | No | No | Biomedical | [ |
12 | PAA/polyvinyl alcohol (PVA)/Agar | Fe3+ | PAA with Fe3+ ions form the 1st network through ionic interaction, the 2nd network formed by the ductile agar polymer and the PVA forms the 3rd network through freeze-thaw method | No | No | Biomedical | [ |
13 | Sodium alginate (SA)/ Poly(AM-co-AA) | Fe3+ | Dual formation: Fe3+-carboxylate ionic interactions and the entanglement between SA and (AM-co-AA) polymer chains. | No | No | Biomedical | [ |
14 | Acrylamide/Acrylic acid | Fe3+ | Hydrophobic association of acrylic acids groups form first crosslinking with Fe3+ coordination and the 2nd occurs due to soaking in water | No | No | Biomedical | [ |
15 | PAA/PVA | Fe3+ | PAA was cross-linked through chemical/ionic further intercalation of PVA results in interpenetrating networks | No | No | Biomedical (Strain and pressure sensors) | [ |
16 | Acrylamide (AM)/Sodium acrylate / PVA-borax | Na+ | Reversible cross-links of PVA and sodium tetraborate via di-ol formation and covalent chemical cross-links from AM‐co‐NaA | No | No | Biomedical | [ |
17 | Sodium alginate (SA)/CMC | Ca2+, Bi3+ | Ca2+ used for SA-CMC and then Bi3+ was used both as drug as well as cross-linker | E. coli | No | Drug delivery | [ |
18 | Guanosine monophosphate (GMP) | Ca2+, Fe3+ | GMP self-assembly forming highly ordered structures with G-quadruplexes are cross-linked by Fe3+ and Ca2+ ions to form double cross-linked hydrogels | HeLa cells | No | Drug delivery | [ |
19 | Poly(AAm-2-AMPS/SA (acrylamido-2-methyl-1-propanesulfonic acid) | Ca2+ | P(AAm-2-AMPS) forms the covalent chemical and the Ca2+ ions cross-link SA | No | No | Skin T.E | [ |
20 | Chitosan/Acrylamide | Fe3+ | CS-PAAm dual network formed by ionic coordination and then covalent using chemical (Bis) | No | Rat | Biomedical | [ |
21 | Alginate/Guar gum | Fe3+ | Glutaraldehyde used for chemical crosslinking and ionic coordination between polydopamine, SA, and Fe3+ | No | No | Biomedical(strain-sensitive, flexible sensor) | [ |
22 | PVA/PAA/Agar | Fe3+, Al3+ | PAA and Agar with ionic coordination with Fe3+ and Al3+ and PVA as interpenetrating polymer to form triple network | E. coli, S. aureus bacteria | No | Antibacterial | [ |
23 | PVA/ Poly(vinyl pyrrolidone) (PVP)/ PAA | Zn2+ | The 1st network between PAA-Zn2+ through metal-coordination and free radical polymerization, followed by PVP as the 2nd network and the 3rd, PVA network via freeze-thaw cycle. | No | No | Cartilage T.E | [ |
24 | P(AAc-co-AAm)/Hydroxypropylated polyrotaxane (HPR) /pullulan | Fe3+ | Free radical polymerization linking of AAc and AAm and then followed by HPR or pullulan and finally with Fe3+ ion complexes | No | No | Cartilage T.E | [ |
Table 1 In vitro and in vivo studies on metal ion cross-linked polymer hydrogels and their biomedical applications.
S.No. | Polymers | Metal Ions | Mechanism | In vitro studies | In vivo studies | Application | Ref |
---|---|---|---|---|---|---|---|
1 | Thiolate/Disulfide exchange | Au+, Ag+ | Thiols and thilolates protection from aerial oxidation with the help of Au and Ag ions by forming Au-S/di-sulphide (SS) (or Ag-S/SS) exchange | Human dermal fibroblasts (HDFs) | No | Potential use as a medical device | [ |
2 | Alginate/CMC | Fe3+ | High electrostatic attractions between carboxylic groups of alginate/CMC and the Fe3+ ions | No | No | Drug delivery | [ |
3 | Plant-origin poly(uronic acid) (PUA) | Fe3+ | Fe3+-polyuronate metal coordination complexes formed from photochemical reaction with visible light irradiation | No | No | Drug delivery | [ |
4 | Poly(dimethyl diallyl ammonium chloride)/Tannic acid (PDDA/TA) | Fe3+ | Multiple pyrogallol TA interacts with PDDA chains through ionic bonds and polymer chains are cross-linked to form networks with the Fe3+ ion coordination | No | No | Other (Adhesion and Cohesion) | [ |
5 | Polygalacturonate | Fe2+ | The galacto-uronate units are cross-linked by interacting with Fe2+ ions | No | No | Biocompatible materials | [ |
6 | Poly(acrylamide-co-acrylic acid) | Fe3+ | The acrylic units are covalently cross-linked and the carboxylate groups and Fe3+ ions form the ionic crosslinking | L929 | No | Biocompatible materials | [ |
7 | Poly(ethylene glycol)- 2,6‐pyridinedicarbonyl (H2pdca)/Poly(acrylic acid) (PAA) | Fe3+ | PEG‐H2pdca form the initial network with metal-ligand interactions. Second network from AA polymerization and cross‐linking through Fe3+ ions | No | No | Electronic skin | [ |
8 | Poly(N-acryloyl glycinamide) PNAGA /Carboxymethyl cellulose (CMC) | Fe3+ | PNAGA cross-linked via hydrogen bonds and CMC cross-linked via Fe3+ ion metal coordination forming dual networks | MTT test | No | Soft T.E | [ |
9 | Polyacrylamide (PAM)/Sodium alginate (SA) | Ag+, Ca2+, Fe3+, Cu2+, Ni2+, Co2+ | For dual network formation PAM/SA was polymerized first and then followed by metal-ion coordination by immersing it in the metal ion solutions and then recovery solutions were used to check the shape recovery. | No | No | Biomedical | [ |
10 | Poly(N,N’-dimethylacrylamide-co-glycidyl methacrylate) (PDMA) | Eu3+ | PDMA consisting of hydrophilic iminodiacetate interacts with lanthanide metal ions dynamically and under stimuli (pH & heating) associate and disassociate | No | No | Biomedical (Biological sensors) | [ |
11 | Xanthan gum | Fe3+ | Coordination bond formation between the Fe3+ ions and the carboxylate groups of xanthan | No | No | Biomedical | [ |
12 | PAA/polyvinyl alcohol (PVA)/Agar | Fe3+ | PAA with Fe3+ ions form the 1st network through ionic interaction, the 2nd network formed by the ductile agar polymer and the PVA forms the 3rd network through freeze-thaw method | No | No | Biomedical | [ |
13 | Sodium alginate (SA)/ Poly(AM-co-AA) | Fe3+ | Dual formation: Fe3+-carboxylate ionic interactions and the entanglement between SA and (AM-co-AA) polymer chains. | No | No | Biomedical | [ |
14 | Acrylamide/Acrylic acid | Fe3+ | Hydrophobic association of acrylic acids groups form first crosslinking with Fe3+ coordination and the 2nd occurs due to soaking in water | No | No | Biomedical | [ |
15 | PAA/PVA | Fe3+ | PAA was cross-linked through chemical/ionic further intercalation of PVA results in interpenetrating networks | No | No | Biomedical (Strain and pressure sensors) | [ |
16 | Acrylamide (AM)/Sodium acrylate / PVA-borax | Na+ | Reversible cross-links of PVA and sodium tetraborate via di-ol formation and covalent chemical cross-links from AM‐co‐NaA | No | No | Biomedical | [ |
17 | Sodium alginate (SA)/CMC | Ca2+, Bi3+ | Ca2+ used for SA-CMC and then Bi3+ was used both as drug as well as cross-linker | E. coli | No | Drug delivery | [ |
18 | Guanosine monophosphate (GMP) | Ca2+, Fe3+ | GMP self-assembly forming highly ordered structures with G-quadruplexes are cross-linked by Fe3+ and Ca2+ ions to form double cross-linked hydrogels | HeLa cells | No | Drug delivery | [ |
19 | Poly(AAm-2-AMPS/SA (acrylamido-2-methyl-1-propanesulfonic acid) | Ca2+ | P(AAm-2-AMPS) forms the covalent chemical and the Ca2+ ions cross-link SA | No | No | Skin T.E | [ |
20 | Chitosan/Acrylamide | Fe3+ | CS-PAAm dual network formed by ionic coordination and then covalent using chemical (Bis) | No | Rat | Biomedical | [ |
21 | Alginate/Guar gum | Fe3+ | Glutaraldehyde used for chemical crosslinking and ionic coordination between polydopamine, SA, and Fe3+ | No | No | Biomedical(strain-sensitive, flexible sensor) | [ |
22 | PVA/PAA/Agar | Fe3+, Al3+ | PAA and Agar with ionic coordination with Fe3+ and Al3+ and PVA as interpenetrating polymer to form triple network | E. coli, S. aureus bacteria | No | Antibacterial | [ |
23 | PVA/ Poly(vinyl pyrrolidone) (PVP)/ PAA | Zn2+ | The 1st network between PAA-Zn2+ through metal-coordination and free radical polymerization, followed by PVP as the 2nd network and the 3rd, PVA network via freeze-thaw cycle. | No | No | Cartilage T.E | [ |
24 | P(AAc-co-AAm)/Hydroxypropylated polyrotaxane (HPR) /pullulan | Fe3+ | Free radical polymerization linking of AAc and AAm and then followed by HPR or pullulan and finally with Fe3+ ion complexes | No | No | Cartilage T.E | [ |
Fig. 2. Schematic representation of gelatin‐ureido‐pyrimidinone (UPy)‐Fe hydrogel crosslinking mechanism (Reprinted with permission from [47] Copyright 2017, Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim).
Fig. 3. Fe-catechol metal-ligand coordination mechanism. (a) The different Fe-catechol forms at varying pH conditions and (b) Fe-catechol trivalent complex and the interaction between catechol groups attached to HA polymer chains.
Fig. 4. Formation of doubly-crosslinked HG-PHs hydrogel from high internal phase emulsions (HIPEs), through metal coordination. (Reprinted with permission from [63] Copyrights 2017, Elsevier Ltd.).
Fig. 5. Schematic representation of the formation of triple network hydrogels using chemical (PAA/Agar) and ionic crosslinking (PAA) and freeze-thaw method (PVA). (Reprinted with permission from [67] Copyright 2018, Elsevier Ltd.).
Fig. 6. Schematic representation of the hydrogel network formation. (a) The molecular structures, stearyl methacrylate (SMA), sodium dodecylbenzene sulfonate (SDBS); (b) hydrogel formation steps. HA gel-hydrophobic association gel, HF gel-ion complex hydrophobic gel, Double physically cross-linked rearranged gels (HFR gels). (Reprinted with permission from [89] Copyright 2018, Elsevier Ltd.).
Fig. 8. (a) Schematic representation of the ionic coordination between the poly(DMA290‐co‐IDHPMA96) and Eu3+ ions. (b) the dynamic metal-ion coordination driving the sol-gel transition and showing the fluorescence switch ON/OFF control. (Reprinted with permission from [107] Copyright 2018, Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim).
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