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Thermoelectric generators are a reliable and environmentally friendly source of electrical energy. A crucial step for their development is the maximization of their efficiency. The efficiency of a TEG is inversely related to its electrical contact resistance, which it is therefore essential to minimize. In this paper, we investigate the contacting of an Al electrode on Mg2(Si,Sn) thermoelectric material and find that samples can show highly asymmetric electrical contact resistivities on both sides of a leg (e.g., 10 µΩ·cm2 and 200 µΩ·cm2). Differential contacting experiments allow one to identify the oxide layer on the Al foil as well as the dicing of the pellets into legs are identified as the main origins of this behavior. In order to avoid any oxidation of the foil, a thin layer of Zn is sputtered after etching the Al surface; this method proves itself effective in keeping the contact resistivities of both interfaces equally low (<10 µΩ·cm2) after dicing. A slight gradient is observed in the n-type leg’s Seebeck coefficient after the contacting with the Zn-coated electrode and the role of Zn in this change is confirmed by comparing the experimental results to hybrid-density functional calculations of Zn point defects.

Mg2(Si,Sn) is an attractive material class due to its excellent thermoelectric (TE) properties, its eco‐friendly constituents, its low mass density, and its low price. A lot of research has been done on optimizing its TE properties; however, works on its use in thermoelectric generators (TEG) are scarce. Herein, the first conversion efficiency measurement of a functional, fully Mg2(Si,Sn)‐based TEG, approaching a maximum value of 4% for an applied ΔT = 375 °C, is shown. A maximum power density of 0.9 W cm−2 (related to the cross‐sectional area of the TE legs) at ΔT=375 °C is also reported, which is among the highest performance of silicide‐based modules reported in literature. Efficiency measurements can be tricky due to the uncertainty of heat flow measurement and parasitic heat losses; therefore, assessing the measurement reliability by confronting it to theoretical calculations is necessary. TEG device simulation in a constant property model is used to compare measured data to expected values and a good match is found (<1% deviation for current at maximum power, <4% difference for maximum power output, deviation within measurement uncertainty range for heat flows and efficiency). The significant discrepancy between measurement and calculations of the inner electrical resistance reveals room for improvement. Cracks form due to thermally induced mechanical stress, which dramatically increase the inner electrical resistance. It is shown that by avoiding those cracks, the maximum power output and conversion efficiency of the TEG could be improved by 30%.

No abstract

α-MgAgSb is a very promising thermoelectric material with excellent thermoelectric properties between room temperature and 300 °C, a range where few other thermoelectric materials show good performance. Previous reports rely on a two-step ball-milling process and/or time-consuming annealing. Aiming for a faster and scalable fabrication route, herein, we investigated other potential synthesis routes and their impact on the thermoelectric properties of α-MgAgSb. We started from a gas-atomized MgAg precursor and employed ball-milling only in the final mixing step. Direct comparison of high energy ball-milling and planetary ball-milling revealed that high energy ball milling already induced formation of MgAgSb, while planetary ball milling did not. This had a strong impact on the microstructure and secondary phase fraction, resulting in superior performance of the high energy ball milling route with an attractive average thermoelectric figure of merit of z T avg = 0.9. We also show that the formation of undesired secondary phases cannot be avoided by a modification of the sintering temperature after planetary ball milling, and discuss the influence of commonly observed secondary phases on the carrier mobility and on the thermoelectric properties of α-MgAgSb.