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Synthesis of Aluminum-Aluminum Nitride Nanocomposites by Gas-Liquid Reactions I. Thermodynamic and Kinetic Considerations

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Abstract

In-situ fabrication of the reinforcing particles directly in the metal matrix is an answer to many of the challenges encountered in manufacturing metal matrix nanocomposite materials. In this method, the nanosized particles are formed directly within the melt by means of a chemical reaction between a specially designed metallic alloy and a reactive gas. The thermodynamic and kinetic characteristics of this chemical reaction dictate the particle size and distribution in the matrix alloy, as well as the nature of the particle/matrix interface, and consequently, they govern many of the material’s mechanical and physical properties. This article focuses on aluminum-aluminum-nitride nanocomposite materials that are synthesized by injecting a nitrogen-bearing gas into a molten aluminum alloy. The thermodynamic and kinetic aspects of the process are modeled, and the detrimental role of oxygen is elucidated.

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Notes

  1. In Eq. [28], coverage (θ) is accounted for in the constant c.

  2. This is a consequence of the drop in the partial pressure of nitrogen inside the bubble, \( P_{{N_{2} ,i}} \), as the bubbles coalesce (Henry’s law).

Abbreviations

\( \alpha_{\text{Li}} \) :

Activation extent of Li in Al-Li alloys at high Li content (>5 pct)

\( \alpha_{\text{Mg}} \) :

Activation extent of Mg in Al-Mg alloys at high Mg content (>5 pct)

\( \gamma \) :

Surface tension of aluminum

\( \delta_{\text{G}} \) :

Thickness of the diffusion layer in the gas bulk

\( \delta_{\text{L}} \) :

Thickness of the diffusion layer in the liquid bulk

η :

Dynamic viscosity of liquid aluminum

θ :

Coverage, defined as \( \theta = \frac{{q_{\text{ads}} }}{{q_{\text{sat}} }} \)

\( \Phi \) :

Measure of the surface drag or velocity gradient at the surface due to the absorbed layer of the gas

µ :

Static viscosity of aluminum

\( \rho_{\text{g}} \) :

Density of gas

\( \rho_{\text{l}} \) :

Density of liquid aluminum

\( A_{\text{t}} \) :

Total gas-liquid interface area

c :

Constant in Eq. [28]

d :

Bubble diameter

\( D_{\text{Al}} \) :

Diffusion coefficient of aluminum

\( D_{\text{N}} \) :

Diffusion coefficient of nitrogen in aluminum

\( d_{\text{o}} \) :

Bubble diameter at bubble detachment

\( d_{\text{no}} \) :

Diameter of the nozzle of the tube

E :

Enhancement factor

\( E_{\text{a}} \) :

Activation energy for chemisorption of nitrogen atoms

\( f_{\text{b}} \) :

Frequency of formation of gas bubbles

He:

Henry’s constant for N2 in liquid Al at T = 1273 K (1000 °C)

\( K_{(12)} \) :

Partition coefficient of Reaction 25

\( K_{\text{AlN}} \) :

Equilibrium constant of Eq. [27]

\( K_{\text{L}} \) :

Mass transfer coefficient of nitrogen in the liquid boundary layer

\( l \) :

Thickness of liquid film in between coalescing bubbles

L :

Depth of the melt

M :

Molar mass of the gas molecule

\( N_{\text{b}} \) :

Number of gas bubbles in the melt

\( P_{\text{GO}} \) :

Pressure of the gas bubble at the moment of detachment from the injection tube

\( P_{\text{l}} \) :

Pressure in the liquid at the injection level

\( P_{{N_{2} ,0}} \) :

Partial pressure of nitrogen in the gas bulk

\( P_{{N_{2} ,i}} \) :

Partial pressure of nitrogen at the gas-liquid interface

\( P_{\text{in}} ,T_{\text{in}} ,V_{\text{in}} \) :

Initial state of reactive gas at the inlet of the injection tube

\( P_{\text{Li}}^{*} \) :

Vapor pressure of pure Li at 1273 K (1000 °C)

\( P_{\text{Mg}}^{*} \) :

Vapor pressure of pure Mg at 1273 K (1000 °C)

\( Q \) :

Gas flow rate

\( q_{\text{ads}} \) :

Occupied adsorption sites on the gas-liquid interface

\( q_{\text{sat}} \) :

Total adsorption sites on the gas-liquid interface

R :

Bubble radius that varies in the melt. R = r at the interface

\( R_{\text{d}} \) :

Radius of the liquid disk between the coalescing bubbles

\( r_{\text{N}} \) :

Rate of chemisorption of nitrogen atoms

T :

Temperature

t :

Gas injection time

\( t_{\text{d}} \) :

Local diffusion time

\( t_{\text{r}} \) :

Residence time of the gas bubble in the melt

\( U_{\text{b}} \) :

Velocity of the gas bubble

\( V_{\text{bo}} \) :

Volume of gas bubble at bubble detachment

\( V_{\text{g}} \) :

Volume of the gas bubble

\( W_{\text{AlN}} \) :

Amount of AlN formed

\( x_{\text{Al}} \) :

Concentration of aluminum

\( x_{{{\text{Al}},i}} \) :

Concentration of aluminum at the gas-liquid interface

\( x_{{{\text{N}},i}} \) :

Concentration of nitrogen atom on the gas-liquid interface

\( x_{{{\text{N}},0}} \) :

Concentration of nitrogen atoms in the liquid bulk

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Authors and Affiliations

  1. Department of Mechanical Engineering, Worcester Polytechnic Institute, Worcester, MA, 01609, USA

    Cecilia Borgonovo (Senior Material Scientist at GKN Hoeganaes Corporations) & Makhlouf M. Makhlouf (Professor)

Authors
  1. Cecilia Borgonovo
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  2. Makhlouf M. Makhlouf
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Correspondence to Makhlouf M. Makhlouf.

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Manuscript submitted December 15, 2015.

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Borgonovo, C., Makhlouf, M.M. Synthesis of Aluminum-Aluminum Nitride Nanocomposites by Gas-Liquid Reactions I. Thermodynamic and Kinetic Considerations. Metall Mater Trans A 47, 5125–5135 (2016). https://doi.org/10.1007/s11661-016-3665-6

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