The factors which influence the formation of solid particles by reaction of sprays with gaseous media were investigated studying the reaction of single macro-drops of orthophosphoric acid with gaseous ammonia. The composition, temperature and physical nature of the drops were measured or recorded as the reaction proceeded. The controlling resistance for mass-transfer was found to exist within the drop and a diffusion model adequately described the uptake of ammonia for the conditions studied. The maximum uptake of ammonia increased with delay in formation of a permanent solid phase. This delay was increased or altered by cyclic exposure of the drop to the gas, humidification of the gas, reduction in acid concentration and addition of sulfuric acid.