Chen Kai-Wei, Zhou Xin-Yu, Dai Xiao-Jun, Chen Yi-Ting, Li Shu-Xuan, Gong Chun-Hui, Wang Peng, Mao Ping, Jiao Yan, Chen Kai, Yang Yi
Jiangsu Key Laboratory of Chemical Pollution Control and Resources Reuse, School of Environmental and Biological Engineering, Nanjing University of Science and Technology, Nanjing 210094, China.
Key Laboratory for Palygorskite Science and Applied Technology of Jiangsu Province, Faculty of Chemical Engineering, Huaiyin Institute of Technology, Huaian 223003, China.
J Hazard Mater. 2024 Jul 15;473:134584. doi: 10.1016/j.jhazmat.2024.134584. Epub 2024 May 11.
Effective capture and immobilization of volatile radioiodine from the off-gas of post-treatment plants is crucial for nuclear safety and public health, considering its long half-life, high toxicity, and environmental mobility. Herein, sulfur vacancy-rich Vs-BiS@C nanocomposites were systematically synthesized via a one-step solvothermal vulcanization of CAU-17 precursor. Batch adsorption experiments demonstrated that the as-synthesized materials exhibited superior iodine adsorption capacity (1505.8 mg g at 200 °C), fast equilibrium time (60 min), and high chemisorption ratio (91.7%), which might benefit from the nanowire structure and abundant sulfur vacancies of BiS. Furthermore, Vs-BiS@C composites exhibited excellent iodine capture performance in complex environments (high temperatures, high humidity and radiation exposure). Mechanistic investigations revealed that the I capture by fabricated materials primarily involved the chemical adsorption between BiS and I to form BiI, and the interaction of I with electrons provided by sulfur vacancies to form polyiodide anions (I). The post-adsorbed iodine samples were successfully immobilized into commercial glass fractions in a stable form (BiOI), exhibiting a normalized iodine leaching rate of 3.81 × 10 g m d. Overall, our work offers a novel strategy for the design of adsorbent materials tailed for efficient capture and immobilization of volatile radioiodine.
考虑到挥发性放射性碘的半衰期长、毒性高和环境迁移性,从后处理厂废气中有效捕获和固定挥发性放射性碘对核安全和公众健康至关重要。在此,通过对CAU-17前驱体进行一步溶剂热硫化,系统地合成了富含硫空位的Vs-BiS@C纳米复合材料。批量吸附实验表明,所合成的材料表现出优异的碘吸附容量(200℃时为1505.8 mg g)、快速平衡时间(60分钟)和高化学吸附率(91.7%),这可能得益于BiS的纳米线结构和丰富的硫空位。此外,Vs-BiS@C复合材料在复杂环境(高温、高湿度和辐射暴露)中表现出优异的碘捕获性能。机理研究表明,所制备材料对碘的捕获主要涉及BiS与I之间的化学吸附形成BiI,以及I与硫空位提供的电子相互作用形成多碘阴离子(I)。吸附后的碘样品成功地以稳定形式(BiOI)固定在商用玻璃碎片中,归一化碘浸出率为3.81×10 g m d。总体而言,我们工作为设计用于高效捕获和固定挥发性放射性碘的吸附材料提供了一种新策略。