This paper presents the general expression for excess virial coefficients o
f binary mixtures in the form of Bartlett's law. Imposing this expression i
n data reduction to determine mixture virial coefficients provides thermody
namically consistent evaluations of cross virial coefficients. Standard dat
a reduction procedures do not provide values of the mixture and cross viria
l coefficients that are both consistent and accurate. We illustrate this ne
w technique by analyzing Burnett data and direct density measurements. In a
ddition, we present the general expression for cross virial coefficients un
der model solution behavior. (C) 1999 Elsevier Science B.V. All rights rese
rved.