Strontium Uptake by Cementitious Materials

Abstract

Wet chemistry experiments and X-ray absorption fine structure (XAFS) measurements were carried out to investigate the immobilization of nonradioactive Sr and 85Sr in calcite-free and calcite-containing Portland cement. The partitioning of pristine Sr between hardened cement paste (HCP) and pore solution, and the uptake of 85Sr and nonradioactive Sr were investigated in batch-type sorption/desorption experiments. Sr uptake by HCP was found to be fast and nearly linear for both cements, indicating that differences in the compositions of the two cements have no influence on Sr binding. The partitioning of pristine Sr bound in the cement matrix and 85Sr between HCP and pore solution could be modeled in terms of a reversible sorption process using similar Kd values. These findings allow 85Sr uptake to be interpreted in terms of an isotopic exchange process with pristine Sr. Sr K-edge EXAFS measurements on Sr doped HCP and calcium silicate hydrate (C-S-H) samples reveal no significant differences in the local coordination environments of pristine Sr and Sr bound to the cement matrix upon sorption. The first coordination sphere consists of five to six oxygen atoms located at a distance of about 2.6 A, which corresponds to Sr-O distances in the hydration sphere of Sr2+ in alkaline solution. Sr binds to the cement matrix via two bridging oxygen atoms located at a distance of about 3.6 A. No further neighboring atoms could be detected, indicating that Sr is taken up as a partially hydrated species by HCP. Wet chemistry and spectroscopic data further indicate that Sr binding to C-S-H phases is likely to be the controlling uptake mechanism in the cement matrix, which allows Sr uptake by HCP to be predicted based on a Ca-Sr ion exchange model previously developed for Sr binding to C-S-H phases. The latter finding suggests that long-term predictions of Sr immobilization in the cementitious near field of repositories for radioactive waste can be based on a simplified sorption model with C-S-H phases.

Cesium and Strontium Retentions Governed by Aluminosilicate Gel in Alkali-Activated Cements

“…The K d values for cesium and strontium obtained in previous studies were sourced from the data in previous studies [35,36,37,38,39,40,41,42,43,44]. It should be noted that the K d value can be influenced by the ratio of the adsorbent to the solution, the concentration of the target ion, the ionic strength of the competing ions, the temperature and the pH; hence, comparison of the K d values can only be done qualitatively.…”

Sorption of strontium on uranyl peroxide: Implications for a high-level nuclear waste repository

“…The fission product Strontium-90 has been considered by the U.S. Environmental Protection Agency as the most important radioactive isotope in the environment [1,2]. Sr-90 is of particular concern because of its high fission yield (from slow-neutron fission of 235 U is 5-6%), its penetrating ionizing radiation (␤ and ␥) during the first several hundreds of years, and its chemical similarity to calcium, which it might follow to its eventual incorporation in human bones [3,4].…”

Theoretical prediction of distribution coefficients of Sr2+ in nuclear waste/ionic liquid phases using COSMO-RS model

“…MOLDEN [38]. The radioactive material used in our computational work was strontium nitrate [Sr(NO 3 [30] and Turbomole 6.2 [31]. In Gaussian03, a frequency optimization was conducted by using the 'freq' keyword by BVP86/TZVP/ DGA1 level of theory [39].…”

“…Among all fission products of nuclear power plants wastes, strontium-90 is considered as the most important radioactive isotope by U.S. Environmental Protection Agency. It has a half-life of 29.1 years and it remains in the environment for a long time after emission [2,3]. It generally exhibits a radioactivity of $0.15 MCi after one year of spent fuel generation [4].…”

“…In such systems, radioactive elements are carried by an acid (e.g. HNO 3 Im] ligands, which can form a coordination complex. These molecules have ring-like structures, where the ring entraps the metal ion and forms a metal complex [29] that resides in the IL-rich phase.…”