Muhire Constantin, Zhang Dongxiang, Chang Cui, Zhang Xu, Li Dagang, Zhiren Guo, Zhang Zilei, Zhang Fengqi, Hou Jinzheng, Li Jinying, Xu Xiyan
School of Chemistry and Chemical Engineering, Beijing Institute of Technology, Beijing 102488, PR China.
School of Chemistry and Chemical Engineering, Beijing Institute of Technology, Beijing 102488, PR China; Department of Chemistry, MSU-BIT University, Shenzhen 517182, PR China.
J Hazard Mater. 2024 Aug 5;474:134688. doi: 10.1016/j.jhazmat.2024.134688. Epub 2024 May 25.
The present work prepared a novel BiMgO-2MBD (X = 0.42) material for iodine vapor capture in temperature conditions related to spent nuclear fuel reprocessing and nuclear accidents. BiMgO-2MBD (X = 0.42) was synthesized by a solvothermal process and exhibited an exceptional ultrafast and high iodine uptake with a capacity of 4352.12 mg/g and 5147.08 mg/g after 5 h at 75 °C and 150 °C, respectively. The TGA analysis shows that Bi/Mg oxide substrate highly contributed to improving the thermal stability of the functionalized BiMgO-2MB (X = 0.42) as indicated by the weight losses of the material components of 3.77 wt%, 29.32 wt%, and 97.72 wt%, respectively for Bi/Mg oxide, BiMgO-2MBD, and 2-MBD. The material characterization and DFT calculations indicate that 2-MBD played a significant role towards improving iodine capture capacity. For long-term and safe waste disposal, a chemically durable waste form was made from etidronic acid and BiO, and successfully immobilized the iodine-loaded wastes (I @BiMgO-2MBD) which exhibited a low normalized leaching rate of 1.098 × 10 g.m/day for 7 days under the PCT-A method. In addition, BiMgO-2MBD (X = 0.42) showed an ability to be reused after several regeneration cycles. The comparison with previously reported materials shows that the current BiMgO-2MBD (X = 0.42) is the first functionalized metal oxide comparable to metal-organic and covalent organic frameworks for iodine uptake. BiMgO-2MBD (X = 0.42) shows promising results for practical applications in the gas phase capture of radioactive iodine.
本研究制备了一种新型的BiMgO-2MBD(X = 0.42)材料,用于在与乏核燃料后处理及核事故相关的温度条件下捕获碘蒸气。BiMgO-2MBD(X = 0.42)通过溶剂热法合成,在75℃和150℃下分别经过5小时后,表现出优异的超快且高碘吸附能力,吸附容量分别为4352.12 mg/g和5147.08 mg/g。热重分析表明,Bi/Mg氧化物基底对提高功能化BiMgO-2MB(X = 0.42)的热稳定性有很大贡献,Bi/Mg氧化物、BiMgO-2MBD和2-MBD的材料组分失重分别为3.77 wt%、29.32 wt%和97.72 wt%。材料表征和密度泛函理论计算表明,2-MBD对提高碘捕获能力起了重要作用。为了实现长期安全的废物处置,由依替膦酸和BiO制成了一种化学耐久性废物形式,并成功固定了载碘废物(I@BiMgO-2MBD),在PCT-A方法下,其7天的归一化浸出率低至1.098×10 g·m/天。此外,BiMgO-2MBD(X = 0.42)在经过几次再生循环后显示出可重复使用的能力。与先前报道的材料相比,当前的BiMgO-2MBD(X = 0.42)是第一种在碘吸附方面可与金属有机框架和共价有机框架相媲美的功能化金属氧化物。BiMgO-2MBD(X = 0.42)在放射性碘的气相捕获实际应用中显示出有前景的结果。