Immobilization of cesium and iodine into Cs3Bi2I9 perovskite-silica composites and core-shell waste forms with high waste loadings and chemical durability

JOURNAL OF HAZARDOUS MATERIALS

卷:401

Article

Yang, Kun¹  Zhu, Weiguang¹  Scott, Spencer²  Wang, Yachun¹  Wang, Jianwei³  Riley, Brian J.⁴  Vienna, John⁴  Lian, Jie¹ 

[1] Rensselaer Polytech Inst, Dept Mech Aerosp & Nucl Engn, Troy, NY 12180 USA

[2] Savannah River Natl Lab, Aiken, SC 29801 USA

[3] Louisiana State Univ, Dept Geol & Geophys, Baton Rouge, LA 70803 USA

[4] Pacific Northwest Natl Lab, Richland, WA 99354 USA

关键词: Pervoskite;    Fission product;    Silica;    Waste form;    Sparking plasma sintering;   

DOI  :  10.1016/j.jhazmat.2020.123279

来源: Elsevier

【 摘 要 】

Cs3Bi2I9, a defect perovskite derivative, is a potential host phase to immobilize iodine and cesium with high waste loadings. In this work, two strategies were explored to form Cs3Bi2I9-silica composites and a core-shell structure in order to improve chemical durability of waste form materials meanwhile maintaining high waste loadings. Cs3Bi2I9 loadings as high as 70 wt.% were incorporated into a silica matrix to form silica-ceramic composites, and 20 wt.% Cs3Bi2I9 was encapsulated into silica to form a core-shell structure by low temperature spark plasma sintering. Chemical durability of the composite and core-shell waste forms was evaluated by semidynamic leaching experiments, and Cs and I were incongruently released from waste form matrices. A BiOI alteration layer formed, acting as a passivation layer to reduce the release of radionuclides. The long-term iodine release rate was low (30 mg m(-2) day 1) for the 70 wt.% Cs3Bi2I9-silica composite leached in deionized water at 90 degrees C, which can be further reduced to 5 x 10(-3) mg m(-2) day(-1) for the 20 wt.% core-shell structure. This work highlights a robust way to immobilize the highly mobile radionuclides with high waste loadings through encapsulation into durable matrices and a surface passivating mechanism that can greatly reduce the elemental transport from waste form materials and significantly enhance their chemical durability.

【 授权许可】

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