The present invention provides methods and compounds for the direct sequestration of chloride ions without requiring the addition of a source of anion such as nitrite or nitrate. A direct sequestration additive is introduced to fresh concrete or hardened concrete where the additive reacts with incoming chloride ions to form a low solubility, chloride-containing compound which captures or sequesters chloride ions. In a preferred embodiment, the chloride-containing compound comprises 3CaO.Fe.sub.(2-x)Al.sub.xO.sub.3.CaCl.sub.2.nH.sub.2O, where x ranges from about 0 to 1.4, and n ranges from about 8 to 24. The chloride ions may be provided in the form of deicing salt or sea water. Because chloride-containing compounds such as 3CaO.Fe.sub.(2-x)Al.sub.xO.sub.3.CaCl.sub.2.nH.sub.2O are formed directly without requiring the addition of a source of anion (e.g. nitrite or nitrate), the process is referred to as "direct sequestration."