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Title: Chalcogenide aerogels as sorbents for radioactive iodine

Journal Article · · Chemistry of Materials, 27(7):2619-2696

Iodine (129I) is one of the radionuclides released in nuclear fuel reprocessing and poses risk to public safety due to its involvement in human metabolic processes. In order to prevent the leaching of hazardous radioactive iodine into the environment, its effective capture and sequestration is pivotal. In the context of finding a suitable matrix for capturing radioactive iodine the chalcogels, NiMoS4, CoMoS4, Sb4Sn4S12, Zn2Sn2S6, and CoSx (x = 4-5) were explored as iodine sorbents. All the chalcogels showed high uptake, reaching up to 225 mass% (2.25 g/g) of the final mass owing to strong chemical and physical iodine-chalcogen interactions. Analysis of the iodine-loaded specimens revealed that the iodine chemically reacted with Sb4Sn4S12, Zn2Sn2S6, and CoSx to form metal complexes SbI3, SnI4, and, KI respectively. The NiMoS4 and CoMoS4 chalcogels did not appear to undergo a chemical reaction with iodine since iodide complexes were not observed with these samples. Once heated, the iodine-loaded chalcogels released iodine in the temperature range of 75 °C to 220 °C, depending on the nature of iodine speciation. In the case of Sb4Sn4S12 and Zn2Sn2S6 iodine release was observed around 150 °C in the form of SnI4 and SbI3, respectively. The NiMoS4, CoMoS4, and CoSx released iodine at ~75 °C, which is consistent with physisorbed iodine. Preliminary investigations on consolidation of iodine-loaded Zn2Sn2S6 with Sb2S3 as a glass forming additive showed the content of iodine in consolidated glass ingots at around 25 mass%.

Research Organization:
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Sponsoring Organization:
USDOE
DOE Contract Number:
AC05-76RL01830
OSTI ID:
1208768
Report Number(s):
PNNL-SA-106676; 600305000
Journal Information:
Chemistry of Materials, 27(7):2619-2696, Journal Name: Chemistry of Materials, 27(7):2619-2696
Country of Publication:
United States
Language:
English

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