摘要
Amorphous zeolite imidazolate framework-8 shows excellent leaching resistance for Eu3+, Th4+, and UO22+ in acidic conditions. • Compressed pores and ion hydrolysis work together to immobilize radionuclides. • A low‑energy, environmentally friendly way that could effectively immobilize Eu3+, Th4+, and UO22+ at room temperature. The proper treatment of high-level liquid waste (HLW) was critical for the sustainability of the nuclear industry. Conventional immobilization methods (glass, cement, and ceramic) had limitations such as high energy consumption, volatile radionuclide release, or waste volume increase. Here, we reported a new strategy to immobilize key radionuclides using zeolitic imidazolate framework-8 (ZIF-8) under high pressure at room temperature, addressing limitations of conventional immobilization. ZIF-8 could be loaded with 10 wt% representative radionuclides (Cs + , Sr 2+ , Eu 3+ , Th 4+ , UO 2 2+ ) and ReO 4 - (a 99 TcO 4 - surrogate), then was amorphized under 1.2 GPa to form glassy ZIF-8 (ZIF-8-G). Finally, after leaching by deionized water or pH = 2 HNO 3 for 42 days, in both leaching solutions, Eu 3+ , Th 4+ , and UO 2 2+ were undetectable, due to their strong interactions with the N-Zn bonds in ZIF-8-G and their hydrolysis into insoluble hydroxides during the heating and loading process, which were then immobilized within ZIF-8-G under high pressure; ≈12% ReO 4 - was leached out because of the larger ionic diameter of ReO 4 - (3∼4 Å)than the pore size of ZIF-8-G (< 3.6 Å); While Cs + and Sr 2+ were completely leached out due to the smaller ionic diameter of Cs + and Sr 2+ (< 3 Å). Compared with conventional immobilization techniques, this technology offers advantages including low-cost raw materials, scalability for large-scale industrial production, simple processing, and environmental friendliness. Download: Download high-res image (281KB) Download: Download full-size image
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