Liu Yang, Shi Feng-Qi, Hao Xin, Li Meng-Yu, Cheng Lin, Wang Cheng, Wang Kai-Yao
Tianjin Key Laboratory of Advanced Functional Porous Materials, Institute for New Energy Materials and Low-Carbon Technologies, School of Materials Science and Engineering, Tianjin University of Technology, Tianjin 300384, PR China.
College of Chemistry, Tianjin Normal University, Tianjin 300387, PR China.
J Hazard Mater. 2023 Sep 15;458:132038. doi: 10.1016/j.jhazmat.2023.132038. Epub 2023 Jul 11.
Efficient adsorption of radioactive Cs and Co and their decay products Ba and Ni bears significance for hazard elimination in case of nuclear emergency, which relies on the adsorption rate enhancement that takes advantages of compositional and structural optimization. Herein, we report a zinc-doped selenidostannate constructed from T2-supertetrahedral clusters, namely K(CHNH)(NH)ZnSnSe·3.4 HO (ZnSnSe-1K). The soft Se and micro-porosity synergistically endow this material with a binding affinity to Cs, Ba, Co, and Ni ions and ultrafast kinetics with R > 97.6% in 2-60 min. In particular, ZnSnSe-1K can remove 99.34% of Cs in 2 min K > 1.5 × 10 mL g), contributing to a record rate constant k of 9.240 g mg min that surpasses all metal chalcogenide adsorbents. ZnSnSe-1K exhibits good acid/base tolerance (pH = 0-12), and the adsorption capacities at neutral are 253.61 ± 9.15, 108.94 ± 25.32, 45.76 ± 14.19 and 38.49 ± 2.99 mg g for Cs, Ba, Co, and Ni, respectively. The adsorption performances resist well co-existing cations and anions, and the removal rates can keep above or close to 90% even in sea water. ZnSnSe-1K is employed in continuous column and membrane filtration, both of which shows excellent elimination efficiency (R > 99%) for mixed Cs, Ba, Co, and Ni. Especially, the membrane with an ultrathin (70 µm) ZnSnSe-1K layer can remove 97-100% Cs in suction filtration with a short contact time of 0.33 s. Combined with the simple synthesis, facile elution and great irradiation resistance, ZnSnSe-1K emerges as a selenide adsorbent candidate for use in environmental remediation especially that involving nuclear waste disposal.
高效吸附放射性铯(Cs)和钴(Co)及其衰变产物钡(Ba)和镍(Ni)对于消除核应急情况下的危害具有重要意义,这依赖于利用成分和结构优化来提高吸附速率。在此,我们报道了一种由T2-超四面体簇构建的锌掺杂硒锡酸盐,即K(CHNH)(NH)ZnSnSe·3.4 HO(ZnSnSe-1K)。柔软的硒和微孔协同赋予该材料对Cs、Ba、Co和Ni离子的结合亲和力以及超快动力学,在2 - 60分钟内去除率R>97.6%。特别是,ZnSnSe-1K在2分钟内可去除99.34%的Cs(K>1.5×10 mL g),其记录速率常数k为9.240 g mg min,超过了所有金属硫族化物吸附剂。ZnSnSe-1K表现出良好的酸碱耐受性(pH = 0 - 12),中性条件下对Cs、Ba、Co和Ni的吸附容量分别为253.61±9.15、108.94±25.32、45.76±14.19和38.49±2.99 mg g。该吸附性能能很好地抵抗共存的阳离子和阴离子,即使在海水中去除率也能保持在90%以上或接近90%。ZnSnSe-1K用于连续柱和膜过滤,两者对混合的Cs、Ba、Co和Ni都显示出优异的去除效率(R>99%)。特别是,具有超薄(70 µm)ZnSnSe-1K层的膜在0.33 s的短接触时间的抽滤中可去除97 - 100%的Cs。结合简单的合成、简便洗脱和良好的抗辐照性,ZnSnSe-1K成为一种用于环境修复特别是涉及核废料处理的硒化物吸附剂候选材料。