Amino-functionalized POSS nanocage-intercalated titanium carbide (Ti_3C_2T_x) MXene stacks for efficient cesium and strontium radionuclide sequestration

摘要

In this work, we prepared two-dimensional (2D) stack-structured aminopropyllsobutyl polyhedral oligomeric silsesquioxane (POSS-NH2) intercalated titanium carbide (Ti3C2Tx) MXene material (Ti3C2Tx/POSS-N-2) using a post-intercalation strategy as a potential adsorbent for the removal of cesium (Cs+) and strontium (Sr2+) ions from aqueous solutions. Ti3C2Tx/POSS-NH2 exhibited unprecedented adsorption capacities of 148 and 172 mg g(-1) for Cs+ and Sr2+ ions, respectively. Batch adsorption experimental data well fitted the Freundlich isotherm model, which revealed multilayer adsorption of Cs+ and Sr2+ ions onto heterogeneous -OH, -F, -O, and -NH2 adsorption sites of Ti3C2Tx/POSS-NH2 with different energies. Ti3C2Tx/POSS-NH2 exhibited rapid Cs+/Sr2+ ions adsorption kinetics and attained equilibrium within 30 min. Also, Ti3C2Tx/POSS-NH2 exhibited recyclable capability over three cycles and remarkable selectivities of 89% and 93% for Cs+ and Sr2+ ions, respectively, in the presence of co-existing mono- and divalent cations. We suggest the high adsorption capacity of Ti3C2Tx/POSS-NH2 might be due to the synergistic effects of (i) increased inter-lamellar distance between Ti3C2Tx galleries due to POSS-NH2 intercalation, enabling diffusion and encapsulation of large numbers of Cs+/Sr2+ ions, (ii) strong complexation of amine (-NH2) groups of POSS-NH2 with Cs+/Sr2+ 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+ /Sr2+ 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 Sr2+ ions from aqueous media.