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The Nopal I uranium deposit of the Sierra Pena Blanca, Mexico, has been the focus of numerous studies because of its economic importance and its use as a natural analog for nuclear-waste disposal in volcanic tuff. Secondary uranyl minerals such as uranophane, Ca[(UO2)(SiO3OH)](2)(H2O)(5), and weeksite, (K,Na)(2)[(UO2)(2)(Si5O13)](H2O)(3), Occur in the vadose zone of the deposit and are overgrown by silica glaze. These glazes consist mainly of opal A, which contains small particles of uraninite, UO2, and weeksite. Close to a fault between brecciated volcanic rocks and welded tuff, a greenish silica glaze coats the altered breccia. Yellow silica glazes from the center or the breccia pipe and from the high-grade pile coat uranyl-silicates, predominantly uranophane and weeksite. All silica glazes are strongly zoned with respect to U and Ca, and the distribution of these elements indicates Curved features and spherical particles inside the coatings. The concentrations of U and Ca Correlate in the different zones and both elements inversely correlate with the concentration of Si. Zones within the silica glazes contain U and Ca in a 1:1 ratio with maximum concentrations of 0.08 and 0.15 at.% for the greenish and yellow glazes, respectively, suggesting trapping of either Ca1U1-aqueous species or -particles in the colloidal silica. X-ray photoelectron spectroscopy (XPS), Fourier-transform infra-red spectroscopy (FTIR), and oxygen-isotope ratios measured by secondary-ion mass spectrometry (SIMS) indicate higher U6+/U4+ ratios, higher proportions of Si-OH groups and lower delta O-18 values for the greenish silica glaze than for the yellow silica glaze. These differences in composition reflect increasing brecciation, porosity, and permeability from the center of the breccia pipe (yellow silica glaze) toward the fault (green silica glaze), where the seepage of meteoric water and Eh are higher. (C) 2009 Elsevier Ltd. All rights reserved.