J. Mater. Sci. Technol. ›› 2020, Vol. 57: 204-220.DOI: 10.1016/j.jmst.2020.03.060
• Invited Review • Previous Articles
Jufeng Huanga, Guang-Ling Songa,b,c,*(), Andrej Atrensc, Matthew Darguschc
Received:
2019-12-16
Published:
2020-11-15
Online:
2020-11-20
Contact:
Guang-Ling Song
Jufeng Huang, Guang-Ling Song, Andrej Atrens, Matthew Dargusch. What activates the Mg surface—A comparison of Mg dissolution mechanisms[J]. J. Mater. Sci. Technol., 2020, 57: 204-220.
Mechanism | Key points | Supporting experiments | Opposing observations |
---|---|---|---|
(1) Partially protective surface film | The surface film increasingly disrupted with increasing current density or potential. | The Mg(OH)2 and MgO on the Mg surface detected [ | The corrosion potential too positive in a neutral or acidic solution [ |
(2) Uni-positive Mg+ ion | Mg electrochemically anodized into univalent Mg+ ion and then immediately reacted chemically with water, converting into Mg2+ and producing hydrogen. | The calculated valence of dissolved Mg was in the range from 1.33 to 1.66 [ | Uni-positive Mg+ ion not experimentally observed by disk-ring electrode [ |
(3) Magnesium hydride (MgH2) | Mg electrochemically or chemically reduced to the hydride and reacted chemically with water to release hydrogen. | MgH2 detected by X-ray diffraction [ | MgH2 more difficult to form under stronger anodic polarization, and thus failure to interpret the NDE [ |
(4) Particle undermining | Particles undermined by corrosion of the surrounding matrix and falling out, resulting in more mass loss than electrochemical dissolution. | A SEM photomicrograph showing a particle partially undermined [ | Hydrogen evolution rate not increased by anodic polarization [ |
(5) Incomplete film univalent Mg+ ion | Analyzed/discussed in detail in the following sections. | ||
(6) Self-corrosion | A self-corrosion process within a crevice (or crack-like feature) isolated by hydrogen bubbles involved in the dissolution of Mg. | Hydrogen bubbles trapped on the surface of corroding Mg [ | The self-corrosion independent from polarization, and thus not responsible for NDE. |
(7) Cathodic catalytic activity | Analyzed/discussed in detail in following sections. |
Table 1 Proposed Mg corrosion and NDE mechanisms.
Mechanism | Key points | Supporting experiments | Opposing observations |
---|---|---|---|
(1) Partially protective surface film | The surface film increasingly disrupted with increasing current density or potential. | The Mg(OH)2 and MgO on the Mg surface detected [ | The corrosion potential too positive in a neutral or acidic solution [ |
(2) Uni-positive Mg+ ion | Mg electrochemically anodized into univalent Mg+ ion and then immediately reacted chemically with water, converting into Mg2+ and producing hydrogen. | The calculated valence of dissolved Mg was in the range from 1.33 to 1.66 [ | Uni-positive Mg+ ion not experimentally observed by disk-ring electrode [ |
(3) Magnesium hydride (MgH2) | Mg electrochemically or chemically reduced to the hydride and reacted chemically with water to release hydrogen. | MgH2 detected by X-ray diffraction [ | MgH2 more difficult to form under stronger anodic polarization, and thus failure to interpret the NDE [ |
(4) Particle undermining | Particles undermined by corrosion of the surrounding matrix and falling out, resulting in more mass loss than electrochemical dissolution. | A SEM photomicrograph showing a particle partially undermined [ | Hydrogen evolution rate not increased by anodic polarization [ |
(5) Incomplete film univalent Mg+ ion | Analyzed/discussed in detail in the following sections. | ||
(6) Self-corrosion | A self-corrosion process within a crevice (or crack-like feature) isolated by hydrogen bubbles involved in the dissolution of Mg. | Hydrogen bubbles trapped on the surface of corroding Mg [ | The self-corrosion independent from polarization, and thus not responsible for NDE. |
(7) Cathodic catalytic activity | Analyzed/discussed in detail in following sections. |
Fig. 4. Schematic Evans diagram explaining the NDE behavior by the exchange of current density for HER [42]. The bold line represents the HE current density as a function of potential.
Species | Oxidation state | State | μ0 (kcal/mol) |
---|---|---|---|
Mg | 0 | Solid | 0 |
Mg+ | +1 | Ion | -61 |
Mg2+ | +2 | Ion | -109 |
Mg(OH)2 | +2 | Solid | -199 |
MgH | +1 | Gas | +34 |
MgH2 | +2 | Solid | -8 |
MgO | +2 | Solid | -136 |
Table 2 Values of the standard Gibbs energy of formation of species [63].
Species | Oxidation state | State | μ0 (kcal/mol) |
---|---|---|---|
Mg | 0 | Solid | 0 |
Mg+ | +1 | Ion | -61 |
Mg2+ | +2 | Ion | -109 |
Mg(OH)2 | +2 | Solid | -199 |
MgH | +1 | Gas | +34 |
MgH2 | +2 | Solid | -8 |
MgO | +2 | Solid | -136 |
Fig. 5. Electrochemical impedance diagrams of Mg in a 0.1 mol/L Na2SO4 solution: (a) after different immersion times at Ecorr, (b) at Ecorr and for two anodic over potentials [55].
Fig. 6. Polarization curves and hydrogen evolution results for Mg in saturated Mg(OH)2 solution: (a) experimental and IR-corrected potentiostatic polarization curves, (b) average hydrogen evolution rates at different potentials, and (c) hydrogen evolution volume versus time at different potentials [81].
Fig. 7. Hydrogen evolution and corrosion morphologies of a polarized Mg alloy MEZU under different polarization conditions, in which (a)-(e) show the cloudy “trails’’ of hydrogen bubbles and trapped hydrogen bubbles associated with cathodic hydrogen evolution, and (d) and (e) show the cloudy zones along the edges of the dark (corroding) areas associated with anodic hydrogen evolution: (a) the alloy at the cathodic potential -1.8 V/SCE; (b) MEZU at a cathodic potential -1.7 V/SCE in the same area as (a); (c) MEZU at anodic potential -1.4 V/SCE in the same area as (a); (d) MEZU at anodic potential -1.4 V/SCE in another area; (e) MEZU at cathodic potential -2 V/SCE in the same area as (d) after anodically polarized at -1.4 V/SCE [17,39].
Fig. 8. Corrosion development on an MEZU specimen during immersion in a 5 % NaCl solution (the faint cloudy “trails” from some small sites in these micrographs are evolving hydrogen bubbles. The cloud “trails” are designated as “cathodic hydrogen evolution”, and denoted as “cathodic” in Fig. 8(a). Some cloudy zones along the edge of the black areas in these figures also involving hydrogen bubbles, and the areas that are black in color are corroded or corroding sites. The hydrogen evolution from these corroding areas is designated “anodic hydrogen evolution” and denoted as “anodic” in Fig. 8(a) [39].
Fig. 9. Hydrogen evolution rates of a pure Mg specimen in 0.1 M HCl galvanostatically polarized at an anodic current density for 10 min., and immediately potentiostatically polarized at cathodic potential -2.2 V vs. Ag/AgCl for 10 min., then the anodic-cathodic step polarization repeated at a more positive anodic current density until 60 mA/cm2 (the anodic hydrogen evolution rate in each the anodic polarization step decreases first and then increases with increase anodic current density, while the cathodic hydrogen evolution rate in the cathodic potentostatic potential -2.2 V (Ag/AgCl) step immediately after the anodic polarization decreases as the anodic current density in the anodic polarization step increases) [These experimental results were recently obtained in the lab].
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