There is major environmental interest in finding a sustainable solution to immobilize ¹²⁹I, a by-product of the nuclear industry. The use of aluminoborosilicate glasses represents a good compromise. However, this solution does not appear adequate for ¹²⁹I owing to its volatility at high temperature during the vitrification process. In the present work, we use a high-pressure (1.5 GPa) apparatus to synthesize I-rich aluminoborosilicate glasses. We show that the use of high-pressure conditions enhances the I solubility in glasses by several orders of magnitude as compared to 1 bar synthesis, with I solubility up to 5.7 mol%. We observed that I is more solubilized in Na-rich as compared to Ca-rich glass. Investigation of the I speciation using XPS also reveals that I solubility in glasses is much higher as I dissolves as I⁵⁺ in comparison to I⁻. Our work shows that using high-pressure appears to be a reliable solution for dissolving a large quantity of I within the structure of aluminoborosilicate glasses for the conditioning of nuclear waste. We also demonstrate that the oxidized I waste form should be employed to greatly increase I solubility in nuclear waste glasses. Therefore, it represents a potential pathway for solving the immobilization of ¹²⁹I produced by anthropic nuclear activity.

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高压条件下合成的核废料玻璃基质中 129I 的固定化：实验研究

寻找一种可持续的解决方案来固定核工业的副产品¹²⁹ I具有重大的环境意义。使用铝硼硅酸盐玻璃是一个很好的折衷方案。但是，此解决方案似乎不足以满足¹²⁹I 由于其在玻璃化过程中在高温下的挥发性。在目前的工作中，我们使用高压 (1.5 GPa) 装置合成富含 I 的铝硼硅酸盐玻璃。我们表明，与 1 bar 合成相比，高压条件的使用将 I 在玻璃中的溶解度提高了几个数量级，I 溶解度高达 5.7 mol%。我们观察到，与富钙玻璃相比，I 更易溶于富钠玻璃。使用 XPS 对 I 形态的研究还表明，与 I ^-相比，I在玻璃中的溶解度要高得多，因为 I 溶解为 I ⁵⁺. 我们的工作表明，使用高压似乎是在铝硼硅酸盐玻璃结构中溶解大量 I 以调节核废料的可靠解决方案。我们还证明应采用氧化的 I 废物形式来大大增加 I 在核废料玻璃中的溶解度。因此，它代表了解决人为核活动产生的¹²⁹ I固定化的潜在途径。