Low-cost solder–graphite composite sheets (≥55 vol.% solder), with solder and graphite forming interpenetrating networks to a degree, are excellent thermal interface materials (TIMs). Solders 63Sn-37Pb and 95.5Sn-4Ag-0.5Cu are separately used, with the latter performing better. In composite fabrication, a mixture of micrometer-size solder powder and ozone-treated exfoliated graphite is compressed to form a graphite network, followed by fluxless solder reflow and subsequent hot pressing to form the solder network. The network connectivity (enhanced by ozone treatment) is lower in the through-thickness direction. The electrical conductivity obeys the rule of mixtures (parallel model in-plane and series model through-thickness), with anisotropy 7. Thermal contact conductance ≤26 × 104 W/(m2 K) (with 15-μm-roughness copper sandwiching surfaces), through-thickness thermal conductivity ≤52 W/(m K), and in-plane thermal expansion coefficient 1 × 10−5/°C are obtained. The contact conductance exceeds or is comparable to that of all other TIMs, provided that solder reflow has occurred and the composite thickness is ≤100 μm. Upon decreasing the thickness below 100 μm, the sandwich thermal resistivity decreases abruptly, the composite through-thickness thermal conductivity increases abruptly to values comparable to the calculated values based on the rule of mixtures (parallel model), and the composite–copper interfacial thermal resistivity (rather than the composite resistivity) becomes dominant.
