Many important processes, such as corrosion, contact catalysis, and powder metallurgy, depend in varying degrees on the reaction of gases on the surface of metals. The object of this investigation is to study the mechanism of this type of reaction on single crystals of copper. In this paper (Part I) experiments are described which show that the rate of reaction with oxygen varies greatly with the crystal plane along which the surface is prepared. In Part II experiments will be described which show that catalytic reactions between certain gases on the surface of a single crystal cause rearrangements of the metal atoms in the surface to develop special planes in a manner dependent on the nature of