Capillarity in pressure infiltration: improvements in characterization of high-temperature systems

In the pressure infiltration of metal matrix composites, molten metal is injected under external pressure into a porous preform of the reinforcing material. Equilibrium capillary parameters characterizing wetting for this process are summarized in plots of metal saturation versus applied pressure, also known as drainage curves. Such curves can be measured in our laboratory during a single experiment with an infiltration apparatus designed to track the rate of metal penetration into porous preforms under conditions characteristic of metal matrix composite processing (temperatures in excess of 1000 A degrees C and pressures in the order of 10 MPa). For such measurements to be valid, infiltration of the preform with molten metal must be mechanically quasi-static, i.e., the metal must flow at a rate sufficiently low for the metal pressure to be essentially uniform across the preform at all times. We examine this requirement quantitatively, using a finite-difference model that simulates the unsaturated unidirectional ingress of molten metal into a ceramic particle preform of finite width. We furthermore present improvements in the experimental apparatus developed in our laboratory to measure the entire drainage curve in a single experiment. We compare numerical results with new experimental data for the copper/alumina system to show (i) that pressurization rates sufficiently low for quasi-static infiltration can be produced with this apparatus, and (ii) that taking the relative permeability equal to the saturation yields better agreement with experiment than does the expression originally proposed by Brooks and Corey.

Characterization of capillary forces during liquid metal infiltration

Maryam Bahraini Hasani

This thesis addresses the link between capillarity parameters, i.e. surface tension and contact angle, and the infiltration of porous preforms with molten metal by pressure infiltration The method used is to conduct pressure infiltration experiments of selected preforms with molten aluminum or copper based alloys, and characterize the level and, where relevant, kinetics of metal ingress into the preforms. Several systems are investigated in turn, comprising chemically inert and reactive systems. Capillarity in the infiltration of alumina particulate preforms with copper are investigated by means of infiltration experiments conducted at 1200°C under argon with a low oxygen partial pressure, characteristic of equilibrium with carbon at that temperature. The experiments were run in a gas pressure driven liquid metal infiltration apparatus capable of melting copper under gas pressures up to 20 MPa. Capillarity parameters are extracted from drainage curves that plot the volume fraction of metal in the porous medium vs. the applied pressure. Mercury porosimetry, which is based on the same principle, is also used on similar preforms for comparison. The effect of volume fraction, particle geometry and capillary parameters on the drainage curve are studied and compared with the expression proposed by Brooks and Corey. The influence of the particle volume fraction and capillary parameters characterizing wetting in the two systems is discussed to derive an effective contact angle for wetting of alumina particles by molten metal. The value thus derived agrees with literature data from sessile drop experiments. A new technique is proposed for the direct measurement of capillary forces during infiltration in systems of relevance to the processing of metal matrix composites. A custom-designed device enables dynamic tracking of the molten metal surface while the infiltration apparatus is pressurized. It comprises an LVDT (Linear Variable Differential Transformer) that is fixed to the top of the infiltration machine and whose core is connected via an alumina tube to a graphite plunger that floats atop the liquid metal. Upon pressurization, the floater movement caused by flow of the metal into the preform is tracked by the LVDT. Capable of handling melt temperatures up to 1250°C and infiltration pressures up to 20 MPa, the method is essentially a high-temperature analogue of mercury porosimetry. Its accuracy is demonstrated by comparison with data obtained using other techniques and its use is illustrated with the infiltration of diamond particle preforms by Al and Al-Si alloys at 700°C. The present method for direct measurement of drainage curves during the infiltration process is then used for the characterization of wetting of SiC particle performs by molten aluminum and Al-12.2at%Si. The ceramic particle diameter is varied from 7 µm to 40 µm and infiltration was characterized at 750°C, varying the applied pressure from 0.1 to 10 MPa. From these data, the relevant work of immersion is calculated by comparison to the work exerted by the external gas pressure over the whole saturation range. The thus determined work of immersion is translated in an apparent contact angle during infiltration, which is compared with the values determined by other techniques reported in literature to find good agreement. Kinetics effects in reactive systems such as SiC/Al and graphite/Cu-Cr were studied by direct measurement of the drainage curves varying the pressurization rate and conducting measurements interrupted at a given pressure. In addition to the analysis of the capillarity parameters already used for the non-reactive systems, the data are analyzed by a simple model based on the Brooks-Corey relation allowing to link the triple-line velocity in liquid metal infiltration with the saturation given one characteristic distance. It is found that alloying elements in systems investigated drive infiltration at fixed pressure, but do not assist pressure infiltration. Quite to the contrary, they may even hamper efficient infiltration by blocking narrow channels via formation of reaction products with the preform material.

EPFL2007

High-temperature wettability and thermal conductivity of aluminium nitride reinforced metal matrix composites

Masahiro Kida

Aluminum nitride (AlN) has been applied to various applications, including electronic substrates and packaging, semiconductor production components, wide band gap semiconductor, light-emitting diodes (LED) and acoustic wave devices; at the same time, it is also attractive as a reinforcement in Metal Matrix Composites (MMCs) for thermal management applications with tailored thermal properties. In this thesis, two main subjects are investigated in terms of both the composite processing and its thermal property, namely (i) the high-temperature wettability between AlN and liquid metals and (ii) the thermal conductivity behavior of AlN reinforced metal matrix composites and the associated question of the interface thermal conductance at the AlN/metal interface. High-temperature wettability of AlN particle preforms with pure Al, Cu, Sn and Pb, was investigated by means of drainage curve measurements during pressure infiltration. The measured drainage curves show good agreement with the semi-empirical model in soil science proposed by Brooks and Corey. The total work of immersion, Wi, can be directly calculated by integration of the drainage curves, in turn giving the apparent contact angle during infiltration at high temperature. For Cu, Sn and Pb, the apparent contact angles deduced by integration of experimental drainage curves are in the range 120-140° and agree well with corresponding sessile drop data from the literature. Data for AlN and α-Al2O3 are furthermore similar for both methods of measurement, which results from the presence of a native oxide layer on the AlN particles, which is not eliminated from the particle surface in these systems. For the wettability between AlN/Pb and α-Al2O3/Pb systems, a slight difference is observed and this behavior is attributed to the transformation of the native oxide layer with temperature and the presence of dissolved oxygen in the melt. On the contrary, the wettability of AlN/Al system gives higher value than the sessile drop data measured in vacuum, corresponding rather to the value measured under He-H2 gas at 1373K. This indicates that in the present study there is no elimination of the native oxide layer on the AlN by the formation of Al2O gas, which normally occurs in high vacuum. Moreover, the results of the present technique gradually deviate to the sessile drop data as the initial contact angle gets close or below 90° especially in the α-Al2O3/Al system, suggesting that there is a minimum value, around 105-110°, below which the present infiltration-based contact-angle measurement technique may lose validity. Thermal conductivity behavior of AlN reinforced metal matrix composites produced by pressure infiltration technique has been characterized at both room and elevated temperature in two different microstructural systems, namely (i) particle reinforced system (PRCs) and (ii) partially sintered particle system, i.e., an interpenetrating composite in which the AlN is also a continuous phase (IPCs). The phase contrast of thermal conductivity between AlN (Κd) and matrix metals (Κm) is varied within a range of 0.4

EPFL2008

Characterization of capillary forces during liquid metal infiltration

Maryam Bahraini Hasani

EPFL2007

High-temperature wettability and thermal conductivity of aluminium nitride reinforced metal matrix composites

Masahiro Kida

EPFL2008