J. Mater. Sci. Technol. ›› 2022, Vol. 102: 232-263.DOI: 10.1016/j.jmst.2021.05.078
• Invited Review • Previous Articles Next Articles
Yanhui Caoa,b, Dajiang Zhengc, Fan Zhangd, Jinshan Pand, Changjian Lina,*()
Received:
2021-02-06
Revised:
2021-04-26
Accepted:
2021-05-20
Published:
2021-08-27
Online:
2021-08-27
Contact:
Changjian Lin
About author:
*E-mail address: cjlin@xmu.edu.cn (C. Lin).Yanhui Cao, Dajiang Zheng, Fan Zhang, Jinshan Pan, Changjian Lin. Layered double hydroxide (LDH) for multi-functionalized corrosion protection of metals: A review[J]. J. Mater. Sci. Technol., 2022, 102: 232-263.
Methods | Advantages | Disadvantages |
---|---|---|
Co-precipitation | ♦Flexibility to obtain desired LDH ♦Simple equipment ♦One-step synthesis | ♦Needs further crystallization ♦Formation of insoluble compounds |
Anion-exchange | ♦Mild reaction conditions ♦Avoids the formation of insoluble compounds | ♦Needs precursor (usually LDH-NO3-) prepared by other methods ♦Two-step synthesis ♦Neutral species cannot be intercalated |
Calcination-reconstruction | ♦Take full advantage of structure memory effect ♦Neutral species can be intercalated ♦he original reactant can be LDH intercalated with any anions (eg. CO32-) | ♦The activity of metal oxides determined the reconstruction ♦Needs LDH precursor prepared by other methods ♦Time-consuming |
Hydrothermal method | ♦Simple reactant ♦Easy operation | ♦High temperature ♦Long reaction time |
Table 1 Advantages and disadvantages of the different methods to prepare LDH powder.
Methods | Advantages | Disadvantages |
---|---|---|
Co-precipitation | ♦Flexibility to obtain desired LDH ♦Simple equipment ♦One-step synthesis | ♦Needs further crystallization ♦Formation of insoluble compounds |
Anion-exchange | ♦Mild reaction conditions ♦Avoids the formation of insoluble compounds | ♦Needs precursor (usually LDH-NO3-) prepared by other methods ♦Two-step synthesis ♦Neutral species cannot be intercalated |
Calcination-reconstruction | ♦Take full advantage of structure memory effect ♦Neutral species can be intercalated ♦he original reactant can be LDH intercalated with any anions (eg. CO32-) | ♦The activity of metal oxides determined the reconstruction ♦Needs LDH precursor prepared by other methods ♦Time-consuming |
Hydrothermal method | ♦Simple reactant ♦Easy operation | ♦High temperature ♦Long reaction time |
Fig. 7. Change of current density along with deposition time (i-t curve) at applied potential of-1.7 V in Zn2+/Al3+ solution (reprinted with permission from [76]).
Methods | Advantages | Disadvantages |
---|---|---|
In-situ hydrothermal method | ♦Strong bonding strength ♦Widely used ♦One-step synthesis ♦Controllable film thickness | ♦Limited substrates (eg. Mg. Al) ♦High temperature ♦Special instrument (Autoclave) |
Electrodeposition | ♦Short reaction time ♦On metal substrate with any shape | ♦Weak bonding strength ♦Energy consuming and high cost |
Co-precipitation | ♦Realize the fabrication of LDH films on any metal substrate | ♦Time-consuming ♦Weak bonding strength |
Spin coating | ♦Controlled orientation ♦On any metal substrates ♦Very thin films | ♦Weak bonding strength ♦Specific equipment |
Steaming coating | ♦Environmentally friendly ♦Suitable for preparation LDH films on large-size Mg alloys | ♦Limited to Mg alloy ♦Specific equipment |
Anion-exchange | ♦Production of various functional LDH films | ♦Based on LDH films prepared by other methods |
Table 2 Advantages and disadvantages of the different methods to prepare LDH film.
Methods | Advantages | Disadvantages |
---|---|---|
In-situ hydrothermal method | ♦Strong bonding strength ♦Widely used ♦One-step synthesis ♦Controllable film thickness | ♦Limited substrates (eg. Mg. Al) ♦High temperature ♦Special instrument (Autoclave) |
Electrodeposition | ♦Short reaction time ♦On metal substrate with any shape | ♦Weak bonding strength ♦Energy consuming and high cost |
Co-precipitation | ♦Realize the fabrication of LDH films on any metal substrate | ♦Time-consuming ♦Weak bonding strength |
Spin coating | ♦Controlled orientation ♦On any metal substrates ♦Very thin films | ♦Weak bonding strength ♦Specific equipment |
Steaming coating | ♦Environmentally friendly ♦Suitable for preparation LDH films on large-size Mg alloys | ♦Limited to Mg alloy ♦Specific equipment |
Anion-exchange | ♦Production of various functional LDH films | ♦Based on LDH films prepared by other methods |
Precursor | Examples | Evidence | Refs. |
---|---|---|---|
M(OH)2 | ♦Zn(OH)2: Zn2+ replaced by Al3+ | ♦Dyeing method | [ |
♦Mg(OH)2: Mg2+ replaced by Al3+ | ♦XPS | [ | |
♦Mg(OH)2: Mg2+ replaced by Al3+ | ♦XPS, XRD | [ | |
M(OH)3 | ♦FeOOH: Fe3+ replaced by Mg2+ | ♦Obtaining FeOOH by electrodeposition firstly | [ |
♦MnOOH: Mn3+ replaced by Mg2+ | ♦Obtaining MnOOH by electrodeposition firstly | [ | |
♦Al(OH)3: Al3+ replaced by Zn2+ | ♦XPS, XRD | [ | |
♦Al(OH)3: Al3+ replaced by Mg2+ | ♦XRD, XPS | [ |
Table 3 Published work supporting ion substitution theory and corresponding evidence.
Precursor | Examples | Evidence | Refs. |
---|---|---|---|
M(OH)2 | ♦Zn(OH)2: Zn2+ replaced by Al3+ | ♦Dyeing method | [ |
♦Mg(OH)2: Mg2+ replaced by Al3+ | ♦XPS | [ | |
♦Mg(OH)2: Mg2+ replaced by Al3+ | ♦XPS, XRD | [ | |
M(OH)3 | ♦FeOOH: Fe3+ replaced by Mg2+ | ♦Obtaining FeOOH by electrodeposition firstly | [ |
♦MnOOH: Mn3+ replaced by Mg2+ | ♦Obtaining MnOOH by electrodeposition firstly | [ | |
♦Al(OH)3: Al3+ replaced by Zn2+ | ♦XPS, XRD | [ | |
♦Al(OH)3: Al3+ replaced by Mg2+ | ♦XRD, XPS | [ |
Fig. 15. Schematic representations of (a) an LDH crystallite and LDH films of the crystallites (b) parallel and (c) perpendicular to the substrate (reprinted with permission from [103]).
Fig. 16. Schematic representation of NiAl-LDH-CO3 films prepared from the aged deionized water (left) and CO2-saturated water (right), respectively (reprinted with permission from [102]).
Fig. 23. 3D SVET maps of the AA2024-T3 without and with ZnAl-LDH-NO3, ZnAl-LDH-VOx after 1 month of immersion in 0.05 mol/L NaCl (reprinted with permission from [115]).
Substrate | LDH | Low-surface-energy materials | Refs. |
---|---|---|---|
Mg alloy AZ91D | ZnAl-LDH | stearic acid | [ |
pure Mg | MgMn-LDH | myristic acid | [ |
pure Mg | MgAl-LDH | sodium oleate | [ |
Mg alloy AZ31 | MgAl-LDH | 2H-perfluorodecyltrimethoxysilane (PFDTMS) | [ |
AA6082 alloy | CeMgAl-LDH | 1H, 1H, 2H, 2H perfluorododecyl trichlorosilane (PFDTS) | [ |
AA2099-T83 Al-Cu-Li alloy | Li-Al-LDH | 1H, 1H, 2H, 2H-Perfluorodecyltrimethoxysilane (PFDTMS) | [ |
Mg alloy AZ31 | MgZnAl LDH | lauric acid | [ |
AA6061 alloy | MgAl-LDH | Triethoxy-1H,1H,2H,2H-tridecafluoro-n-octylsilane (FAS-13) | [ |
Pure Al | ZnAl-LDH | sodium laurate | [ |
]Mg alloy AZ80 | MgAl-LDH | polytetrafluoroethylene (PTFE) | [ |
Table 4 Reported superhydrophobic LDH films in the literature.
Substrate | LDH | Low-surface-energy materials | Refs. |
---|---|---|---|
Mg alloy AZ91D | ZnAl-LDH | stearic acid | [ |
pure Mg | MgMn-LDH | myristic acid | [ |
pure Mg | MgAl-LDH | sodium oleate | [ |
Mg alloy AZ31 | MgAl-LDH | 2H-perfluorodecyltrimethoxysilane (PFDTMS) | [ |
AA6082 alloy | CeMgAl-LDH | 1H, 1H, 2H, 2H perfluorododecyl trichlorosilane (PFDTS) | [ |
AA2099-T83 Al-Cu-Li alloy | Li-Al-LDH | 1H, 1H, 2H, 2H-Perfluorodecyltrimethoxysilane (PFDTMS) | [ |
Mg alloy AZ31 | MgZnAl LDH | lauric acid | [ |
AA6061 alloy | MgAl-LDH | Triethoxy-1H,1H,2H,2H-tridecafluoro-n-octylsilane (FAS-13) | [ |
Pure Al | ZnAl-LDH | sodium laurate | [ |
]Mg alloy AZ80 | MgAl-LDH | polytetrafluoroethylene (PTFE) | [ |
Fig. 26. Schematic showing the fabrication of anticorrosion system with self-reparable slippery surface and active corrosion inhibition on PEO modified Mg alloy (reprinted with permission from [164]).
Fig. 29. A scheme describing the synthesis process of reduced graphene oxide/layered double hydroxide (RGO/ZnAl-LDH) film and the anticorrosion mechanism (reprinted with permission from [167]).
Fig. 32. Nyquist plots of carbon steel in mortar with different contents of MgAl-LDHs-NO2- after (a) 2 W/D cycles, (b) 11 W/D cycles and (c) 12 W/D cycles (reprinted with permission from [14]).
Fig. 33. A schematic illustration of the corrosion protection mechanism of MgAl-LDHs-NO2- for steel in concrete (reprinted with permission from [14]).
LDH | Preparation method | Dosage | Age | Mechanical property | Application | Refs. | |||
---|---|---|---|---|---|---|---|---|---|
Compressive strength | Flexural strength | Improve chloride migration resistance | Improve carbonation resistance | Corrosion inhibition | |||||
CaAl-LDH | co-precipitation | 0.5-2% Vol. | 28d | +17% (1% LDH) | +55% (1%LDH) | √ | / | √ | [ |
MgAl-pAB | calcination-rehydration | 5-10% | 28d | -17.2% (10% LDH) | -21% (10% LDH) | √ | / | √ | [ |
MgAl-CO3 | \ | 1,2% | 28d | -6.3% (1% LDH) | / | / | √ | / | [ |
MgAl-LDH | \ | 2-4% | 26d | / | / | / | √ | / | [ |
calcined MgAl-CO3 | \ | 1-3% | 28d | Slight increase | / | / | / | / | [ |
MgAl-LDH | hydrothermal method | 1-3% | 56d | -6.3% (1% LDH) | / | √ | / | / | [ |
MgAl-NO2 | calcination-rehydration | 2-8% | 28d | -9.4% (8% LDH) | -3.1% (8% LDH) | / | / | √ | [ |
MgAl-NO2 | co-precipitation | 2-4% | \ | / | / | √ | / | √ | [ |
ZnAl-NO2 | co-precipitation | 2% | 8d | / | / | √ | / | √ | [ |
Table 5 Reported LDH types and their application in concrete.
LDH | Preparation method | Dosage | Age | Mechanical property | Application | Refs. | |||
---|---|---|---|---|---|---|---|---|---|
Compressive strength | Flexural strength | Improve chloride migration resistance | Improve carbonation resistance | Corrosion inhibition | |||||
CaAl-LDH | co-precipitation | 0.5-2% Vol. | 28d | +17% (1% LDH) | +55% (1%LDH) | √ | / | √ | [ |
MgAl-pAB | calcination-rehydration | 5-10% | 28d | -17.2% (10% LDH) | -21% (10% LDH) | √ | / | √ | [ |
MgAl-CO3 | \ | 1,2% | 28d | -6.3% (1% LDH) | / | / | √ | / | [ |
MgAl-LDH | \ | 2-4% | 26d | / | / | / | √ | / | [ |
calcined MgAl-CO3 | \ | 1-3% | 28d | Slight increase | / | / | / | / | [ |
MgAl-LDH | hydrothermal method | 1-3% | 56d | -6.3% (1% LDH) | / | √ | / | / | [ |
MgAl-NO2 | calcination-rehydration | 2-8% | 28d | -9.4% (8% LDH) | -3.1% (8% LDH) | / | / | √ | [ |
MgAl-NO2 | co-precipitation | 2-4% | \ | / | / | √ | / | √ | [ |
ZnAl-NO2 | co-precipitation | 2% | 8d | / | / | √ | / | √ | [ |
Fig. 37. The Bode (a1) and Nyquist (b1) diagrams of samples soaked for 5 days, the Bode (b1) and Nyquist (b2) diagrams of samples soaked for 25 days, the Bode (c1) and Nyquist (c2) diagrams of samples soaked for 50 days, the Bode (d1) and Nyquist (d2) diagrams of samples soaked for 70 days. (reprinted with permission from [212]).
LDH | Intercalated anions | Preparation method | Substrate | coating | Refs. |
---|---|---|---|---|---|
ZnAlCe-LDH | NO3- | co-precipitation | AA2024 | hybrid sol-gel (SiOx/ZrOx) layer | [ |
ZnAlCe-LDH | MoO42- and V2O74- | co-precipitation+anion exchange | AA2024 | hybrid sol-gel (SiOx/ZrOx) | [ |
ZnAlCe-LDH | vanadate, 2-mercapto benzothiazole, molybdate, phytic acid and 8-hydroxyquinoline | co-precipitation+anion exchange | AA2024-T3 | hybrid sol-gel silica matrix sol | [ |
ZnAl-LDH | PO43- | co-precipitation+anion exchange | Mild steel | silane primer | [ |
GO/LDH | vanadate anions and 2-mercaptobenzothiazole anions (MBT) | co-precipitation+anion exchange | AA2024-T3 | sol-gel coating | [ |
ZnAl-LDH | 2-benzothiazolythio-succinic acid(BTSA) and benzoate (BZ) | coprecipitation | carbon steel | epoxy coating | [ |
MgAl LDH | NO2- | acidification oscillation and ion exchange. | Q235 steel | epoxy coating | [ |
Mg/Al LDH | Methionine | coprecipitation | Mg alloy | epoxy coating | [ |
ZnAl-LDH | Molybdate | coprecipitation | carbon steel | epoxy coating | [ |
MgAl-LDH | F- | co-precipitation+anion exchange | Mg alloy | epoxy resin | [ |
MgA-LDH | benzotriazole (BTA) | coprecipitation | Zn-Mg coated steel | epoxy-based coating | [ |
Table 6 Summary of the published work reporting the application of LDH powder for corrosion protection of various metals.
LDH | Intercalated anions | Preparation method | Substrate | coating | Refs. |
---|---|---|---|---|---|
ZnAlCe-LDH | NO3- | co-precipitation | AA2024 | hybrid sol-gel (SiOx/ZrOx) layer | [ |
ZnAlCe-LDH | MoO42- and V2O74- | co-precipitation+anion exchange | AA2024 | hybrid sol-gel (SiOx/ZrOx) | [ |
ZnAlCe-LDH | vanadate, 2-mercapto benzothiazole, molybdate, phytic acid and 8-hydroxyquinoline | co-precipitation+anion exchange | AA2024-T3 | hybrid sol-gel silica matrix sol | [ |
ZnAl-LDH | PO43- | co-precipitation+anion exchange | Mild steel | silane primer | [ |
GO/LDH | vanadate anions and 2-mercaptobenzothiazole anions (MBT) | co-precipitation+anion exchange | AA2024-T3 | sol-gel coating | [ |
ZnAl-LDH | 2-benzothiazolythio-succinic acid(BTSA) and benzoate (BZ) | coprecipitation | carbon steel | epoxy coating | [ |
MgAl LDH | NO2- | acidification oscillation and ion exchange. | Q235 steel | epoxy coating | [ |
Mg/Al LDH | Methionine | coprecipitation | Mg alloy | epoxy coating | [ |
ZnAl-LDH | Molybdate | coprecipitation | carbon steel | epoxy coating | [ |
MgAl-LDH | F- | co-precipitation+anion exchange | Mg alloy | epoxy resin | [ |
MgA-LDH | benzotriazole (BTA) | coprecipitation | Zn-Mg coated steel | epoxy-based coating | [ |
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