Hollow Bismuth-Based Nanoreactor with Ultrathin Disordered Mesoporous Silica Shell for Superior Radioactive Iodine Decontamination

Zhenjiang Tian, Tien-Shee Chee, Yuxun Hao, Kang Kang, Xiaofan Yang and Chengliang Xiao*, 
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Abstract

The effective removal of radioactive iodine under harsh high-temperature conditions, akin to those encountered in real spent nuclear fuel reprocessing, remains a formidable challenge. Herein, a novel bismuth-based mesoporous silica nanoreactor with a distinctive hollow yolk–shell structure was successfully synthesized by using silica-coated Bi2O3 as a hard template and alkaline organic ammonia for etching (Bi@HMS-1, HMS = hollow mesoporous silica). In contrast to conventional inorganic alkali-assisted methods with organic template agents, our approach yielded a material with thinner and more disordered shell layers, along with a relatively smaller pore volume. This led to a significant reduction in the physisorption of Bi@HMS-1 onto iodine while maintaining a smooth passage of guest iodine molecules into and out of the shell channels. Consequently, the resulting sorbent exhibited an outstanding iodine sorption capacity at high temperatures, achieving a chemisorption percentage as high as 96.5%, which makes it extremely competitive among the currently reported sorbents.

Abstract Image

带有超薄无序介孔二氧化硅壳的中空铋基纳米反应器可实现卓越的放射性碘去污效果
在严酷的高温条件下(类似于实际核乏燃料后处理中遇到的条件)有效去除放射性碘仍然是一项艰巨的挑战。在此,我们以二氧化硅包覆的 Bi2O3 为硬模板,以碱性有机氨水为蚀刻剂,成功合成了具有独特空心蛋壳结构的新型铋基介孔二氧化硅纳米反应器(Bi@HMS-1,HMS = 空心介孔二氧化硅)。与使用有机模板剂的传统无机碱辅助方法相比,我们的方法得到的材料具有更薄、更无序的外壳层,同时孔隙体积相对较小。这大大减少了 Bi@HMS-1 对碘的物理吸附,同时保持了客碘分子进出壳通道的顺畅。因此,所制备的吸附剂在高温下具有出色的碘吸附能力,化学吸附率高达 96.5%,在目前已报道的吸附剂中极具竞争力。
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