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The experimental hydration of obsidian for up to 30 days is described at relative humidities (RH) of 60, 90, 95, and 100 percent and at temperatures of 150, 160, and 175°C. Under isothermal conditions, the rate of hydration increased by as much as 25 percent between 60 and 100 percent RH. The RH dependence is nonlinear, with the majority of the rate increase occurring between 90 and 100 percent RH. The effect of RH can be related to the driving force for molecular water diffusion in obsidians as described by the chemical potential difference between water sorbed onto the obsidian surface and intrinsic water in the obsidian. The differences in hydration rates caused by RH differences in experiments approximate the error commonly described for obsidian-hydration dating. These results suggest that obsidian-hydration dating requires a knowledge of the site temperature and relative humidity in order to accurately generate age estimates.

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Users of the obsidian hydration dating method have routinely assumed that artifacts which originate from the same geological flow will be of the same chemical composition and thus hydrate at the same rate under equivalent conditions of temperature and relative humidity. Recent laboratory experimentation into the hydration process has shown that the intrinsic water content of the glass is the dominant factor in establishing the rate of hydration. Water content determinations on a large suite of samples from numerous prehistoric quarries within the Coso volcanic field, California, indicated that water content values, and thus hydration rate, varied significantly on a within flow basis. It is recommended that water determinations be made on individual artifacts prior to obsidian hydration dating. 0 1993 John Wiley & Sons, Inc.

A program has been established for DOE Environmental Restoration and Waste Management (EM) to evaluate factors that are likely to affect waste glass reaction ,during repository disposal, with emphasis on an unsaturated environment typical of what may be expected for the proposed Yucca Mountain repository site. This report covers progress in FY 1991 on the following tasks: 11 A critic_ review of those parameters that affect the reactivity of glass in an unsaturated environment is in progress. This effort involves a search of the literature to identify the important parameters. Temperature and glass compositions are the first parameters examined in detail. 2, An interface between waste producers and the repository program is being implemented. 3. A series of tests has been started to evaluate the reactivity of fully radioactive glasses in a high-level waste repository environment mad compare it to the reactivity of synthetic glasses of similar composition. 4. The effect of radiation upon the durability of waste glasses at a high glass surface. _ea-tc)-liquid volume fSA/V) _ttio m3d higl_ gas-to-liquid volume ratio will be assessed. These tesLsaddress both vapor m_d high SA/V liquid conditions. 5. A series of test:_ is being performed to compare the extent of reaction (_t" nuclear waste glasses at various SA/V ratios, Such differences in the SA/V ratio may significantly affect glass durability. 6. An_ytical electron microscopy (AEM), infrared spectroscopy, and nuclear : resonant profiling are being used to assess the glass/water reaction pathway by identil'ying intermediate phases that appear on the reacting glass. Additionally, colloids trom the leach solutions are being studied using AEM.