The temporal evolution of natural illite du Puy dissolution rates was measured from Si release rates in single-pass flow-through experiments lasting at least 100 days at 25°C and pH ranging from 2 to 12. Si release rates decreased by a factor of five and three at pH 12 and 2, respectively, during the experiments. These observations are interpreted to stem from changes in illite du Puy reactive surface area during these experiments. As the edges of clay minerals dissolve faster than the basal planes, dissolution tends to change clay mineral morphology decreasing the percentage of reactive edge sites. This continuously changing morphology prevents illite dissolution rates from attaining steady state during laboratory experiments lasting 100 to 200 days. A similar temporal decrease in dissolution rates is evident for many different sets of clay mineral dissolution rate data available in the literature. It seems reasonable, therefore, to expect that clay mineral dissolution does not attain steady state in nature, but rather their dissolution rates decrease continuously during their dissolution.