Tian Zhenjiang, Chee Tien-Shee, Hao Yuxun, Kang Kang, Yang Xiaofan, Xiao Chengliang
College of Chemical and Biological Engineering, Zhejiang University, Hangzhou 310058, P.R. China.
Department of Materials Science and Engineering, Korea Advanced Institute of Science and Technology, Daejeon 34141, South Korea.
Chem Bio Eng. 2024 Apr 16;1(6):548-558. doi: 10.1021/cbe.4c00010. eCollection 2024 Jul 25.
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 BiO 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.
在类似于实际乏核燃料后处理中遇到的苛刻高温条件下,有效去除放射性碘仍然是一项艰巨的挑战。在此,以二氧化硅包覆的BiO为硬模板,用碱性有机氨进行蚀刻,成功合成了一种具有独特中空蛋黄壳结构的新型铋基介孔二氧化硅纳米反应器(Bi@HMS-1,HMS = 中空介孔二氧化硅)。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壳层更薄且无序程度更高,同时孔体积相对较小。这导致Bi@HMS-1对碘的物理吸附显著降低,同时保持客体碘分子能够顺利进出壳层通道。因此,所得吸附剂在高温下表现出出色的碘吸附能力,化学吸附百分比高达96.5%,这使其在目前报道的吸附剂中极具竞争力。