We have investigated the influence of Sc substitution on the transport and magnetic properties of YbAl2, a well-known intermediate valence compound. Sc substitution provides a chemical pressure that decreases the lattice constant and thereby alters the Yb valence as a function of composition and temperature. We observe a strong correlation between the Seebeck coefficient and the ratio of trivalent to divalent Yb in these compounds, as determined from magnetic susceptibility measurements. This correlation indicates that the largest absolute value of the Seebeck coefficient is achieved when the average Yb valence is near 2.5 (the ratio of divalent to trivalent Yb is 1:1). It is shown that Sc concentration can be used as a means to tune both the magnitude of the maximum of the Seebeck coefficient and the temperature at which this absolute maximum occurs, improving the prospects of the use of these materials in cryogenic Peltier coolers.

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