Baskaran Karthikeyan, Elliott Casey, Ali Muhammad, Moon Jeremy, Beland Jade, Cohrs Dave, Chong Saehwa, Riley Brian J, Chidambaram Dev, Carlson Krista
Department of Chemical and Materials Engineering, University of Nevada, Reno, Reno, NV 89557, USA.
Pacific Northwest National Laboratory (PNNL), Richland, WA 99532, USA.
J Hazard Mater. 2023 Mar 15;446:130644. doi: 10.1016/j.jhazmat.2022.130644. Epub 2022 Dec 20.
The capture of long-lived radioactive iodine (I) from oxidizing off-gasses produced from reprocessing used nuclear fuel is paramount to human health and environmental safety. Bismuth has been investigated as a viable iodine getter but the phase stability of bismuth-based sorbents in an oxidizing environment have not yet been researched. In the current work, bismuth nanoparticle-based sorbents, as free particles (Bi-NPs) and embedded within silica xerogel monoliths made with a porogen (TEO-5), were exposed to I before and after aging in 1 v/v% NO at 150 °C. For unaged sorbents, BiI was the dominant phase after iodine capture with 8-30 mass% BiOI present due to native BiO on the surface of the unaged nanoparticles. After 3 h of aging, 82 mass% of the Bi-NPs was converted to BiO with only a small amount of iodine captured as BiOI (18 mass%). After aging TEO-5 for 3 h, iodine was captured as both BiI (26 %) and BiOI (74 %) and no BiO was detected.". Additionally, bismuth lining the micrometer-scale pores in the TEO-5 led to enhanced iodine capture. In a subsequent exposure of the sorbents to NO (secondary aging), all BiI converted to BiOI. Thus, direct capture of iodine as BiOI is desired (over BiI) to minimize loss of iodine after capture.
从乏核燃料后处理产生的氧化性废气中捕获长寿命放射性碘(I)对人类健康和环境安全至关重要。铋已被研究作为一种可行的碘捕获剂,但铋基吸附剂在氧化环境中的相稳定性尚未得到研究。在当前工作中,基于铋纳米颗粒的吸附剂,以自由颗粒(Bi-NPs)形式以及嵌入由致孔剂(TEO-5)制成的二氧化硅干凝胶整体材料中,在150°C下于1 v/v% NO中老化前后均暴露于碘。对于未老化的吸附剂,捕获碘后BiI是主要相,由于未老化纳米颗粒表面存在天然BiO,有8 - 30质量%的BiOI存在。老化3小时后,82质量%的Bi-NPs转化为BiO,仅捕获少量碘作为BiOI(18质量%)。TEO-5老化3小时后,碘以BiI(26%)和BiOI(74%)两种形式被捕获,未检测到BiO。此外,TEO-5中微米级孔隙内衬的铋导致碘捕获增强。在随后吸附剂暴露于NO(二次老化)时,所有BiI都转化为BiOI。因此,期望直接以BiOI形式捕获碘(相对于BiI)以最小化捕获后碘的损失。