These papers, designated I and II, discuss measurements of excess Ba (and/or Sr) in practical oxide coated cathodes. More than 300 cathodes of various designs were prepared, aged for periods up to 50 000 hours, tested thermionically, and then analyzed chemically.Despite its great importance, the accurate measurement of excess Ba in practical cathodes is a problem whose complexity has not been adequately realized. Although the methods of the present experiments avoided many difficulties, limitations still exist. The difficulties and limitations, as well as the capabilities, can best be discussed in terms of typical measurements; we emphasize this aspect in I.