Amino-functionalized POSS nanocage-intercalated titanium carbide (Ti3C2Tx) MXene stacks for efficient cesium and strontium radionuclide sequestration

纳米笼 吸附 插层(化学) 材料科学 水溶液 倍半硅氧烷 核化学 化学 无机化学 物理化学 有机化学 催化作用 聚合物
作者
Muruganantham Rethinasabapathy,Seung Kyu Hwang,Sung-Min Kang,Changhyun Roh,Yun Suk Huh
出处
期刊:Journal of Hazardous Materials [Elsevier]
卷期号:418: 126315-126315 被引量:33
标识
DOI:10.1016/j.jhazmat.2021.126315
摘要

In this work, we prepared two-dimensional (2D) stack-structured aminopropylIsobutyl polyhedral oligomeric silsesquioxane (POSS-NH 2 ) intercalated titanium carbide (Ti 3 C 2 T x ) MXene material (Ti 3 C 2 T x /POSS-NH 2 ) using a post-intercalation strategy as a potential adsorbent for the removal of cesium (Cs + ) and strontium (Sr 2+ ) ions from aqueous solutions. Ti 3 C 2 T x /POSS-NH 2 exhibited unprecedented adsorption capacities of 148 and 172 mg g −1 for Cs + and Sr 2+ ions, respectively. Batch adsorption experimental data well fitted the Freundlich isotherm model, which revealed multilayer adsorption of Cs + and Sr 2+ ions onto heterogeneous –OH, –F, –O, and –NH 2 adsorption sites of Ti 3 C 2 T x /POSS-NH 2 with different energies. Ti 3 C 2 T x /POSS-NH 2 exhibited rapid Cs + /Sr 2+ ions adsorption kinetics and attained equilibrium within 30 min. Also, Ti 3 C 2 T x /POSS-NH 2 exhibited recyclable capability over three cycles and remarkable selectivities of 89% and 93% for Cs + and Sr 2+ ions, respectively, in the presence of co-existing mono- and divalent cations. We suggest the high adsorption capacity of Ti 3 C 2 T x /POSS-NH 2 might be due to the synergistic effects of (i) increased inter-lamellar distance between Ti 3 C 2 T x galleries due to POSS-NH 2 intercalation, enabling diffusion and encapsulation of large numbers of Cs + /Sr 2+ ions, (ii) strong complexation of amine (–NH 2 ) groups of POSS-NH 2 with Cs + /Sr 2+ ions, and (iii) the presence of large numbers of heterogeneous surface functional groups (e.g., –OH, –F, and –O), which resulted in the adsorptions of Cs + /Sr 2+ ions through electrostatic, ion exchange, and surface complexation mechanisms. Given the extraordinary adsorption capacities observed, intercalation appears to be a promising strategy for the effective removal of radioactive Cs + and Sr 2+ ions from aqueous media. • Unprecedented Cs + and Sr 2+ adsorption of Ti 3 C 2 T x MXene through POSS-NH 2 intercalation. • Strong complexation of –NH 2 groups of POSS-NH 2 with Cs + and Sr 2+ ions. • Intercalation increases Ti 3 C 2 T x interlayer distance and encapsulates more Cs and Sr. • Adsorption via synergistic electrostatic, complexation, and ion exchange processes. • Maximum Cs + and Sr 2+ adsorption capacities of 148 and 172 mg g −1 , respectively.
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