材料科学与技术 ›› 2018, Vol. 34 ›› Issue (9): 1455-1466.DOI: 10.1016/j.jmst.2018.03.003
所属专题： Biomaterials 2018
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收稿日期:2017-12-19修回日期:2018-02-04接受日期:2018-02-05出版日期:2018-09-20发布日期:2018-09-25
Layered double hydroxide coatings on magnesium alloys: A review
Lian Guoa, Wei Wua, Yongfeng Zhoua, Fen Zhanga*(
), Rongchang Zenga*(), Jianmin Zengb
- a College of Material Science and Engineering, Shandong University of Science and Technology, Qingdao 266590, China
b Ministry-Province Jointly-constructed Cultivation Base for State Key Laboratory of Processing for Non-ferrous Metal and Featured Materials, Guangxi University, Nanning 530004, China
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Received:2017-12-19Revised:2018-02-04Accepted:2018-02-05Online:2018-09-20Published:2018-09-25 -
Contact:Zhang Fen,Zeng Rongchang
引用本文
. [J]. 材料科学与技术, 2018, 34(9): 1455-1466.
Lian Guo, Wei Wu, Yongfeng Zhou, Fen Zhang, Rongchang Zeng, Jianmin Zeng. Layered double hydroxide coatings on magnesium alloys: A review[J]. J. Mater. Sci. Technol., 2018, 34(9): 1455-1466.
Fig. 1. Schematic illustration of LDH structure and chemical components [48].
Fig. 1. Schematic illustration of LDH structure and chemical components [48].
Fig. 2. Solutions used in the two-step in situ method.
Fig. 2. Solutions used in the two-step in situ method.
Fig. 3. Forming mechanism of Mg-Al LDH film [80].
Fig. 3. Forming mechanism of Mg-Al LDH film [80].
Fig. 4. Temperature and time of in situ methods on Mg alloys.
Fig. 4. Temperature and time of in situ methods on Mg alloys.
Fig. 5. SEM micrographs of bare Mg (a), top of Mg-Al LDH/Mg alloy (b), (c) and cross cutting (d) [87].
Fig. 5. SEM micrographs of bare Mg (a), top of Mg-Al LDH/Mg alloy (b), (c) and cross cutting (d) [87].
Fig. 6. A schematic illustration of the apparatus used to electrochemically fabricate Li-Al LDH thin film on AZ31, with DC voltage being applied between steel pipe (the anode) and AZ31 sample (the cathode) in Li+/Al3+ aqueous electrolyte [91].
Fig. 6. A schematic illustration of the apparatus used to electrochemically fabricate Li-Al LDH thin film on AZ31, with DC voltage being applied between steel pipe (the anode) and AZ31 sample (the cathode) in Li+/Al3+ aqueous electrolyte [91].
Fig. 7. TEM image of LDH powder sample scraped from spin coated LDH film prepared with a single coating step [95].
Fig. 7. TEM image of LDH powder sample scraped from spin coated LDH film prepared with a single coating step [95].
Fig. 8. Schematic illustration of the formation process of ZnAl-VOx LDH and ZnAl-Cl LDH films on Mg alloy. Step I: fabrication ZnAl-NO3 LDH films by a facile hydrothermal crystallization method. ZnAl-NO3 LDH display a layered structure built from stacking of brucite-type cationic slabs intercalated nitrate anions and water molecules. Step II: formation of ZnAl-VOx LDHs and ZnAl-Cl LDH films via anion exchange process [96].
Fig. 8. Schematic illustration of the formation process of ZnAl-VOx LDH and ZnAl-Cl LDH films on Mg alloy. Step I: fabrication ZnAl-NO3 LDH films by a facile hydrothermal crystallization method. ZnAl-NO3 LDH display a layered structure built from stacking of brucite-type cationic slabs intercalated nitrate anions and water molecules. Step II: formation of ZnAl-VOx LDHs and ZnAl-Cl LDH films via anion exchange process [96].
Fig. 9. Ratios of synthetic methods of LDH coatings on Mg alloys.
Fig. 9. Ratios of synthetic methods of LDH coatings on Mg alloys.
Table 1 Advantages and disadvantages of the different synthetic methods.
| Methods | Advantages | Disadvantages |
|---|---|---|
| In situ growth | ? Ease of operation ? Strong adhesion ? Controllable size | ? Substrate as only source ? Time consuming ? Highly temperature |
| Co-precipitation | ? Controllable chemical compositions ? Wide scope of application ? Ease of operation | ? Time consuming ? Weak adhesion |
| Electrochemical deposition | ? Purity of phase ? High deposition rate ? Simple equipment ? Complex shapes | ? Complex operation ? High cost |
| Spinning coating | ? Ease of operation ? Very thin films | ? High cost ? Weak adhesion |
| Anion-exchange | ? Ease of operation ? Diverse intercalation ions | ? Low crystallinity ? Time consuming |
Table 1 Advantages and disadvantages of the different synthetic methods.
| Methods | Advantages | Disadvantages |
|---|---|---|
| In situ growth | ? Ease of operation ? Strong adhesion ? Controllable size | ? Substrate as only source ? Time consuming ? Highly temperature |
| Co-precipitation | ? Controllable chemical compositions ? Wide scope of application ? Ease of operation | ? Time consuming ? Weak adhesion |
| Electrochemical deposition | ? Purity of phase ? High deposition rate ? Simple equipment ? Complex shapes | ? Complex operation ? High cost |
| Spinning coating | ? Ease of operation ? Very thin films | ? High cost ? Weak adhesion |
| Anion-exchange | ? Ease of operation ? Diverse intercalation ions | ? Low crystallinity ? Time consuming |
Table 2 Thickness and corrosion resistance of the different LDH coatings.
| Method | substrate | LDH coatings | Thickness (μm) | electrolyte | icorr (A/cm2) substrate | icorr (A/cm2) LDH coating | Ref. |
|---|---|---|---|---|---|---|---|
| one-step in situ growth method | AZ91D | MgAl-CO32- | 5-8 | 3.5?wt.% NaCl | 2?×?10-4 | 10-5 | [ |
| one-step in situ growth method | Pure Mg | MgFe-CO32- | 2 | R-SBF | 4.23?×?10-4 | 1.4?×?10-5 | [ |
| two-step in situ growth method | AZ31 | MgAl-CO32- | 1.04 | 0.1?M NaCl | 5.94?×?10-5 | 4.53?×?10-6 | [ |
| hydrothermal treatment | AZ91D | MgAl-CO32- | 25 | 3.5?wt.% NaCl | 4.7?×?10-6 | 1.13?×?10-7 | [ |
| hydrothermal treatment | JDBM | MgAl-CO32- | 2.6 | 3.5?wt.% NaCl | 1.56?×?10-5 | 3.63?×?10-7 | [ |
| urea hydrolysis | AZ31 | MgAl-CO32- | 25-50 | 3.5?wt.% NaCl | 3.4?×?10-5 | 5.75?×?10-6 | [ |
| urea hydrolysis | pure Mg | MgAl-CO32- | 3 | 3.5?wt.% NaCl | 10-4 | 10-6 | [ |
| Steam coating | AZ31 | MgAl-CO32- | 80 | 5?wt.% NaCl | 1.20?×?10-4 | 1.35?×?10-10 | [ |
| Steam coating | AZ31 | MgAl-CO32- | 28.13 | 0.86?M NaCl | 3.46?×?10-5 | 1.24?×?10-9 | [ |
| hydrothermal crystallization method | AZ31D | MgAl-CO32- | 20 | 3.5?wt.% NaCl | 5.24?×?10-6 | 1.46?×?10-6 | [ |
| co-precipitation and hydrothermal method | AZ31 | MgAl-CO32- | 7 | 3.5?wt.% NaCl | 3.04?×?10-5 | 6.52?×?10-8 | [ |
| co-precipitation and hydrothermal method | AZ31 | MgAl-MoO42- | 17 | 3.5?wt.% NaCl | 3.17?×?10-5 | 1.60?×?10-7 | [ |
| electrochemical deposition | AZ31 | LiAl-CO32- | ～0.82 | 0.1?M NaCl | 1.33?×?10-5 | 1.46?×?10-6 | [ |
| electrochemical deposition | AZ91D | ZnAl-NO3- | 3 | 3.5?wt.% NaCl | 4.23?×?10-5 | 2.12?×?10-6 | [ |
| Spinning coating | AZ31 | MgAl-CO32- | 1.1 | 3.5?wt.% NaCl | 1.94?×?10-4 | 4.91?×?10-6 | [ |
| Anion-exchange | AZ91D | ZnAl-Cl- | ～4.7 | 3.5?wt.% NaCl | 6.42?×?10-4 | 2.52?×?10-6 | [ |
| Anion-exchange | AZ91D | ZnAl-VOx- | ～5.2 | 3.5?wt.% NaCl | 6.42?×?10-4 | 2.21?×?10-6 | [ |
Table 2 Thickness and corrosion resistance of the different LDH coatings.
| Method | substrate | LDH coatings | Thickness (μm) | electrolyte | icorr (A/cm2) substrate | icorr (A/cm2) LDH coating | Ref. |
|---|---|---|---|---|---|---|---|
| one-step in situ growth method | AZ91D | MgAl-CO32- | 5-8 | 3.5?wt.% NaCl | 2?×?10-4 | 10-5 | [ |
| one-step in situ growth method | Pure Mg | MgFe-CO32- | 2 | R-SBF | 4.23?×?10-4 | 1.4?×?10-5 | [ |
| two-step in situ growth method | AZ31 | MgAl-CO32- | 1.04 | 0.1?M NaCl | 5.94?×?10-5 | 4.53?×?10-6 | [ |
| hydrothermal treatment | AZ91D | MgAl-CO32- | 25 | 3.5?wt.% NaCl | 4.7?×?10-6 | 1.13?×?10-7 | [ |
| hydrothermal treatment | JDBM | MgAl-CO32- | 2.6 | 3.5?wt.% NaCl | 1.56?×?10-5 | 3.63?×?10-7 | [ |
| urea hydrolysis | AZ31 | MgAl-CO32- | 25-50 | 3.5?wt.% NaCl | 3.4?×?10-5 | 5.75?×?10-6 | [ |
| urea hydrolysis | pure Mg | MgAl-CO32- | 3 | 3.5?wt.% NaCl | 10-4 | 10-6 | [ |
| Steam coating | AZ31 | MgAl-CO32- | 80 | 5?wt.% NaCl | 1.20?×?10-4 | 1.35?×?10-10 | [ |
| Steam coating | AZ31 | MgAl-CO32- | 28.13 | 0.86?M NaCl | 3.46?×?10-5 | 1.24?×?10-9 | [ |
| hydrothermal crystallization method | AZ31D | MgAl-CO32- | 20 | 3.5?wt.% NaCl | 5.24?×?10-6 | 1.46?×?10-6 | [ |
| co-precipitation and hydrothermal method | AZ31 | MgAl-CO32- | 7 | 3.5?wt.% NaCl | 3.04?×?10-5 | 6.52?×?10-8 | [ |
| co-precipitation and hydrothermal method | AZ31 | MgAl-MoO42- | 17 | 3.5?wt.% NaCl | 3.17?×?10-5 | 1.60?×?10-7 | [ |
| electrochemical deposition | AZ31 | LiAl-CO32- | ～0.82 | 0.1?M NaCl | 1.33?×?10-5 | 1.46?×?10-6 | [ |
| electrochemical deposition | AZ91D | ZnAl-NO3- | 3 | 3.5?wt.% NaCl | 4.23?×?10-5 | 2.12?×?10-6 | [ |
| Spinning coating | AZ31 | MgAl-CO32- | 1.1 | 3.5?wt.% NaCl | 1.94?×?10-4 | 4.91?×?10-6 | [ |
| Anion-exchange | AZ91D | ZnAl-Cl- | ～4.7 | 3.5?wt.% NaCl | 6.42?×?10-4 | 2.52?×?10-6 | [ |
| Anion-exchange | AZ91D | ZnAl-VOx- | ～5.2 | 3.5?wt.% NaCl | 6.42?×?10-4 | 2.21?×?10-6 | [ |
Fig. 10. Schematic representation showing treatment process assisted by alternating electric field: (a-c) in 10?g/L Ce(NO3)3 solution and (d-f) in 30?g/L Ce(NO3)3 solution [104].
Fig. 10. Schematic representation showing treatment process assisted by alternating electric field: (a-c) in 10?g/L Ce(NO3)3 solution and (d-f) in 30?g/L Ce(NO3)3 solution [104].
Fig. 11. SEM morphologies of prepared (a-c) ZnAl-LDH coating and (d-f) LDH/PLA coating [110].
Fig. 11. SEM morphologies of prepared (a-c) ZnAl-LDH coating and (d-f) LDH/PLA coating [110].
Fig. 12. SEM surface morphology images at low and higher magnifications of anodized and Mg-M LDHs, (a) and (b) anodized Mg alloy, (c) and (d) Mg-Fe LDHs, (e) and (f) Mg-Cr LDHs, (g) and (h) Mg-Al LDHs [123].
Fig. 12. SEM surface morphology images at low and higher magnifications of anodized and Mg-M LDHs, (a) and (b) anodized Mg alloy, (c) and (d) Mg-Fe LDHs, (e) and (f) Mg-Cr LDHs, (g) and (h) Mg-Al LDHs [123].
Table 3 Thickness and corrosion resistance of the composite coatings.
| Coatings | Thickness (μm) | electrolyte | icorr (A/cm2) substrate | icorr (A/cm2) LDH | icorr (A/cm2) composite coatings | Ref. |
|---|---|---|---|---|---|---|
| PA/LDH/AZ31 | 0.965 | 3.5?wt.% NaCl | 5.94?×?10-5 | 4.53?×?10-6 | 7.6?×?10-7 | [ |
| Ce(NO3)3/LDH/AZ91D | ～9.7 | 3.5?wt.% NaCl | - | 5.40?×?10-5 | 1.53?×?10-6 | [ |
| PLA/LDH/AZ31 | 7.5 | 3.5?wt.% NaCl | 3.37?×?10-5 | 6.79?×?10-8 | 1.20?×?10-8 | [ |
| LDH/PEO/AZ31 | 7 | 3.5?wt.% NaCl | 1.66?×?10-5 | 3.34?×?10-5 | 3.92?×?10-6 | [ |
| SA/LDH/AZ91D | - | 3.5?wt.% NaCl | 8.8?×?10-3 | 1.1?×?10-3 | 2.6?×?10-5 | [ |
| SA/LDH/AZ31 | 7.5 | 3.5?wt.% NaCl | 4.7?×?10-5 | 3.9?×?10-7 | 3.4?×?10-10 | [ |
| PFOTES/LDH/AZ80 | 5 | 3.5?wt.% NaCl | 1.22?×?10-5 | 0.55?×?10-7 | 3.35?×?10-9 | [ |
| Mg-Al LDH/anodic AZ31 | ～14 | 3.5?wt.% NaCl | 3.27?×?10-5 | 4.70?×?10-6 | 1.18?×?10-7 | [ |
| Mg-Fe LDH/anodic AZ31 | ～14 | 3.5?wt.% NaCl | 3.27?×?10-5 | 4.70?×?10-6 | 1.09?×?10-6 | [ |
| Mg-Cr LDH/anodic AZ31 | ～14 | 3.5?wt.% NaCl | 3.27?×?10-5 | 4.70?×?10-6 | 2.16?×?10-6 | [ |
| LDH/anodic AZ31 | 1.9 | 3.5?wt.% NaCl | 1.23?×?10-5 | 2.85?×?10-6 | 3.5?×?10-7 | [ |
| NO3- LDH/anodic AZ31 | 8 | 3.5?wt.% NaCl | 1.23?×?10-5 | 3.89?×?10-6 | 9.48?×?10-7 | [ |
| VO3- LDH/anodic AZ31 | 8 | 3.5?wt.% NaCl | 1.23?×?10-5 | 3.89?×?10-6 | 2.48?×?10-7 | [ |
Table 3 Thickness and corrosion resistance of the composite coatings.
| Coatings | Thickness (μm) | electrolyte | icorr (A/cm2) substrate | icorr (A/cm2) LDH | icorr (A/cm2) composite coatings | Ref. |
|---|---|---|---|---|---|---|
| PA/LDH/AZ31 | 0.965 | 3.5?wt.% NaCl | 5.94?×?10-5 | 4.53?×?10-6 | 7.6?×?10-7 | [ |
| Ce(NO3)3/LDH/AZ91D | ～9.7 | 3.5?wt.% NaCl | - | 5.40?×?10-5 | 1.53?×?10-6 | [ |
| PLA/LDH/AZ31 | 7.5 | 3.5?wt.% NaCl | 3.37?×?10-5 | 6.79?×?10-8 | 1.20?×?10-8 | [ |
| LDH/PEO/AZ31 | 7 | 3.5?wt.% NaCl | 1.66?×?10-5 | 3.34?×?10-5 | 3.92?×?10-6 | [ |
| SA/LDH/AZ91D | - | 3.5?wt.% NaCl | 8.8?×?10-3 | 1.1?×?10-3 | 2.6?×?10-5 | [ |
| SA/LDH/AZ31 | 7.5 | 3.5?wt.% NaCl | 4.7?×?10-5 | 3.9?×?10-7 | 3.4?×?10-10 | [ |
| PFOTES/LDH/AZ80 | 5 | 3.5?wt.% NaCl | 1.22?×?10-5 | 0.55?×?10-7 | 3.35?×?10-9 | [ |
| Mg-Al LDH/anodic AZ31 | ～14 | 3.5?wt.% NaCl | 3.27?×?10-5 | 4.70?×?10-6 | 1.18?×?10-7 | [ |
| Mg-Fe LDH/anodic AZ31 | ～14 | 3.5?wt.% NaCl | 3.27?×?10-5 | 4.70?×?10-6 | 1.09?×?10-6 | [ |
| Mg-Cr LDH/anodic AZ31 | ～14 | 3.5?wt.% NaCl | 3.27?×?10-5 | 4.70?×?10-6 | 2.16?×?10-6 | [ |
| LDH/anodic AZ31 | 1.9 | 3.5?wt.% NaCl | 1.23?×?10-5 | 2.85?×?10-6 | 3.5?×?10-7 | [ |
| NO3- LDH/anodic AZ31 | 8 | 3.5?wt.% NaCl | 1.23?×?10-5 | 3.89?×?10-6 | 9.48?×?10-7 | [ |
| VO3- LDH/anodic AZ31 | 8 | 3.5?wt.% NaCl | 1.23?×?10-5 | 3.89?×?10-6 | 2.48?×?10-7 | [ |
Fig. 13. Development history of LDH coatings on Mg alloys.
Fig. 13. Development history of LDH coatings on Mg alloys.
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