Spherulitic Lead Calcium Apatite Minerals in Lead Water Pipes Exposed to Phosphate-Dosed Tap Water

Phosphate dosing is the principle strategy used in the United Kingdom to reduce the concentration of lead in tap waters supplied by lead water pipes. The mechanisms of phosphate-mediated lead control are not fully understood, but solid solutions of lead calcium apatite are thought to play an important role. This study investigated the microstructure of a lead pipe, supplied with high-alkalinity tap water, in which the lead calcium apatite crystals were spherulitic having rounded and dumb-bell-shaped morphologies. XRD, Fourier transform infrared spectroscopy, optical microscopy, Raman spectroscopy, scanning electron microscopy, and energy-dispersive spectroscopy showed that the lead pipe had a well-established inner layer of litharge; a middle layer containing lead calcium apatite spherulites, plumbonacrite, and some hydrocerussite; and an outer layer containing iron, lead, phosphorus, calcium, silicon, and aluminum. It was found that spherulitic lead calcium apatite could be grown in the laboratory by adding hydrocerussite to synthetic soft and hard water-containing phosphate, chloride, and citrate ions at pH 5.5 but not when the citrate was absent. This suggests that dissolved organic molecules might play a role in spherulite formation on lead water pipes. These molecules might inhibit the formation of lead calcium apatite, reducing the effectiveness of phosphate dosing in lead water pipes.