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SCIENCE CHINA Materials, Volume 64 , Issue 9 : 2093-2106(2021) https://doi.org/10.1007/s40843-020-1661-1

Advances in layer-by-layer self-assembled coatings upon biodegradable magnesium alloys

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  • ReceivedAug 6, 2020
  • AcceptedMar 5, 2021
  • PublishedMay 27, 2021

Abstract


Funded by

the National Natural Science Foundation of China(52071191)

Shandong University of Science and Technology(SDUST)

and the Science and Technology Innovation Fund of SDUST for graduate students(SDKDYC180371)


Acknowledgment

This work was supported by the National Natural Science Foundation of China (52071191), Shandong University of Science and Technology (SDUST) Research Fund (2014TDJH104) and the Science and Technology Innovation Fund of SDUST for graduate students (SDKDYC180371).


Interest statement

The authors declare that they have no conflict of interest.


Contributions statement

He LJ and Shao Y wrote the paper with support from Zeng RC. Li SQ, Ji XJ, Zhao YB and Cui LY modified this review article. All authors contributed to the final version of the manuscript.


Author information

Li-Jun He received her BE degree from Shandong University of Science and Technology in 2019 and is now a PhD candidate at the university. Her research interest is mainly focused on the design and construction of layer-by-layer assembly functional coating.


Yang Shao received his BE degree from Shandong University of Science and Technology in 2019 and is now a MS student at the university. His research mainly covers biomedical metal surface modification, corrosion and protection of metals.


Shuo-Qi Li is an associate professor at the College of Materials Science and Engineering, Shandong University of Science and Technology. He received his PhD degree from Beijing Normal University in 2012. His research is mainly concentrated on layer-by-layer self-assembled coatings on biodegradable magnesium alloys.


Rong-Chang Zeng is currently a professor at the College of Materials Science and Engineering, Shandong University of Science and Technology. He received his PhD degree from the Institute of Metal Research, Chinese Academy of Sciences in 2003. He is currently editorial board member of Bioactive Materials, Journal of Magnesium and Alloys, and Frontiers of Materials Science, etc. His research interest is focused on corrosion and protection of metals, biodegradable magnesium alloys and surface functionalized modification.


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  • Figure 1

    Schematic representation of the key factors in LbL assembly on Mg alloys.

  • Figure 2

    The possible interactions in the LbL assembly. Reprinted with permission from Ref. [34]. Copyright 2014, American Chemical Society.

  • Figure 3

    Schematic diagram of the LbL assembly of polyelectrolytes on Mg alloy surface by dip coating.

  • Figure 4

    Illustration of fabrication processing of LbL self-assembled coatings using dip (a), spin (b) and spray-assisted methods (c). Reprinted with permission from Ref. [78]. Copyright 2020, Elsevier Ltd.

  • Figure 5

    Two types of spraying: (a) alternate spraying and (b) simultaneous spraying. Reprinted with permission from Ref. [87]. Copygight 2014, The Royal Society of Chemistry.

  • Figure 6

    Potential medical requirements that could be achieved LbL self-assembly.

  • Figure 7

    Schematic illustration of the corrosion mechanism of the Mg alloy (a) and coated Mg alloy (b).

  • Figure 8

    Schematic diagram of the multilayer coating-modified Mg alloy for inhibiting the colonization of bacteria via contact-killing and release-killing.

  • Figure 9

    Schematic representation of the preparation of (PAA/GS)20/PAA-HAp coating. Reprinted with permission from Ref. [123]. Copyright 2019, Elsevier Ltd.

  • Table 1   LbL self-assembled coatings of Mg alloys surface with electrostatic force

    Materials

    Multilayer film

    Polycation

    Polyanion

    Ref.

    AZ91D Mg alloy

    (PEI/PSS/8HQ/PSS)n

    PEI

    PSS

    [38]

    AZ31 Mg alloy

    (PEI/PLGA or PCL/PAH)n

    PEI, PAH

    PLGA or PCL

    [31]

    Mg-3Zn-0.5Sr alloy

    CS-HP-n

    CS-Gel (TiO2)

    HPs

    [49]

    AZ31 Mg alloy

    (CIP/PAH/SiO2/PAH)n

    PAH

    CIP

    [50]

    AZ31B Mg alloy

    (GOCS/Hep)n

    GOCS

    Hep

    [52]

    Mg-1Zn alloy

    (bPEI/GO/bPEI/PA)10

    bPEI

    GO,PA

    [53]

    AZ31D Mg alloy

    [P(DOP)-co-P(DMAEMA+)/DS-Ag]n

    P(DOP)-co-P(DMAEMA+)

    DS-Ag

    [54]

  • Table 2   Comparison of advantages and disadvantages of four intermolecular forces

    Molecular interaction

    Advantage

    Disadvantage

    Ref.

    Electrostatic interaction

    Fabrication process performed in aqueous solution, which is relatively simple; wide selection of assembly materials, and not limited by size, shape, type; coating thickness and properties can be precisely controlled

    Only applicable to assembly of charged PELs in aqueous solution; it is easy to be affected by ion strength and other factors during assembly process, and the detection procedure is expensive, which requires high accuracy of the instrument

    [4043,4648]

    Covalent bonding

    The coating has good stability and resistance to external pH, temperature and ionic strength; different functional groups can be assembled into the coating effectively; the assembly process can occur not only in aqueous solutions but also in organic solvents

    Different assembled molecules may react with each other, bringing impurities to the coating; low output, complicated and expensive methodology

    [6669]

    Hydrogen bonding

    Functional molecules with no charge can be assembled by hydrogen bond; it could prepare layered and erasable polymer multilayers; ensure high directionality and structural diversity

    LbL-assembled multilayer films prepared with this driving force have lower binding force and less stability than other intermolecular interactions; easily affected by pH value and temperature

    [58,70,71]

    Charge transfer interaction

    Multilayer films can be achieved by assembling nonionic molecules; can be assembled in organic solvents; multilayer film is easily detected by spectroscopic technique

    Limited to electron donating and accepting groups of non-ionic molecules

    [65,72,73]

  • Table 3   Electrochemical parameters of multilayer coatings on AZ31 Mg alloy

    Coating

    Solution

    Thickness (µm)

    Ecorr (V/SCE)

    icorr (µA cm−2)

    Ref.

    Substrate

    Coating

    Substrate

    Coating

    (PVP/DNA)20

    SBF

    −1.74

    −1.53

    84.30

    4.71

    [90]

    (Chi/HGO)5

    SBF

    0.755

    −1.801

    −1.376

    88.63

    0.7483

    [92]

    CeO2/(PEI/CMC@GO)10

    3.5% NaCl

    −1.539 

    −1.406 

    53.96

    5.071

    [96]

    EGCG a/Mg

    SBF b

    24.5 + 0.6

    −1.39

    −1.45

    16.20

    0.104

    [97]

    (SiO2/CeO2)10

    HBSS c

    0.630

    −1.463±0.006

    −1.366±0.016

    8.073±0.221

    0.758±0.105

    [98]

    EGCG: epigallocatechin gallate; b) SBF: simulated body fluid; c) HBSS: Hank's Balanced Salt Solution.

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