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• An efficient and economic HDPy-bent material was synthesized and applied for removing 99Tc from contaminated water. 99Tc is one of the critical fission products in the treatment of wastewater and the nuclear waste repository due to its long half-life (t 1/2 = 2.13 × 105 y), high fission yield (~6%), and high mobility in the environment. The development of highly-efficient, low-cost and easily available materials that can rapidly and selectively remove 99Tc is of great significance, but remains a challenge. In this work, bentonite-based materials (HDPy-bent) were obtained through modifying bentonite with hexadecylpyridinium (HDPy) and applied for the remove of TcO 4 − as well as its surrogate ReO 4 −. The structure of HDPy-bent (e.g., the values of d 001) was evaluated and the maximum loading amount of HDPy on bentonite was found to be 200% CEC. The loaded HDPy+ might replace exchangeable cations in the inter-layer space of bentonite. Batch experiment results show that HDPy-bent could quantitatively remove TcO 4 − from aqueous solution within 3 min. The distribution coefficient (K d) of TcO 4 − in this material is up to 2.1 × 105 mL/g, which is significantly higher than most of the previously tested inorganic adsorbent materials. More importantly, HDPy-bent can selectively remove TcO 4 − in the presence of large excess (80,000 times) of competitive anions (NO 3 –, SO 4 2−, CO 3 2−, PO 4 3− and Cl−). This work demonstrates that the HDPy-bentonite is a low cost, and effective adsorbent for removing 99Tc from contaminated water. [ABSTRACT FROM AUTHOR]

Efficient and cost-effective removal of radioactive iodine anions from contaminated water has become a crucial task and a great challenge for waste treatment and environmental remediation. Herein, we present hexadecylpyridinium chloride monohydrate modified bentonite (HDPy-bent) for the efficient and selective removal of iodine anions (I− and IO 3 −) from contaminated water. Batch experiments showed that HDPy-bent could remove more than 95% of I− and IO 3 − within 10 min, and had maximum I− and IO 3 − adsorption capacities of 80.0 and 50.2 mg/g, respectively. Competitive experiments indicated that HDPy-bent exhibited excellent I− and IO 3 − selectivity in the excessive presence of common concomitant anions including PO 4 3−, SO 4 2−, HCO 3 −, NO 3 −, Cl− (maximum mole ratio of anions vs iodine anions was ∼50,000). An anion exchange mechanism was proposed for the selective adsorption of iodine anions. Optimal adsorption structure of HDPy+/I− (IO 3 −) at atomic level and driving forces of the I− (IO 3 −) adsorption were calculated by density functional theory (DFT) simulations. Moreover, the good durability and reusability of the HDPy-bent has been demonstrated with 5 adsorption-desorption cycles. Dynamic column experiment also demonstrated that HDPy-bent exhibited excellent removal and fractional recovery capabilities towards I− and IO 3 − from simulated groundwater and environmental water samples. In conclusion, this work presents a promising adsorbent material for the decontamination of radioactive iodine anions from wastewater on a large scale. [Display omitted] • HDPy-bent showed excellent adsorption abilities for iodide and iodate. • Anions exchange mechanism was confirmed by batch experiments and DFT simulations. • The pyridine N was the intrinsic active site of the modified bentonite. • HDPy-bent was efficient for removing radioiodine anions from wastewater. [ABSTRACT FROM AUTHOR]