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[Display omitted] • HDPy-bent with high adsorption capacity and fast kinetic for 99TcO 4 − was synthesized. • HDPy-bent displayed superior selectivity towards 99TcO 4 −. • Adsorption mechanism of anion exchange and surface precipitation was confirmed by experiments and DFT simulations. • HDPy-bent was proved to be an excellent material for 99Tc decontamination from wastewater by successful column experiments. Technetium-99 (99Tc), as one of the important high-yield fission products, poses a significant threat to the environment and human health due to its radiotoxicity, long half-life, high solubility and mobility in the environment. Thus, removal of 99TcO 4 − from radioactive wastewater is considerably imminent for waste disposal and environment conservation. In this work, Hexadecylpyridinium Chloride Monohydrate modified bentonite (HDPy-bent) was synthesised and used as an adsorbent to remove 99TcO 4 −. The adsorption behaviours of ReO 4 − as an analogue for TcO 4 − were investigated as functions of contact time, solution pH, initial concentration, and competing anions using batch techniques. It is demonstrated that the HDPy-bent showed an excellent adsorption ability for ReO 4 − at the pH range of 2–11, fast adsorption kinetic (reaching equilibrium within 3 min at room temperature), and maintains desirable ReO 4 − adsorption in the presence of concomitant anions at an excessive concentration of 500 times (Cl−, HCO 3 −, NO 3 −, CO 3 2−, SO 4 2− and PO 4 3−). As for adsorption mechanism, we propose the anion exchange process at low concentration of Re(VII) and precipitation reaction at high concentration, while the driving force of the high ReO 4 − adsorption ability is the interaction between ReO 4 − anion and pyridinium ring of HDPy+, which is confirmed by density functional theory (DFT) simulations. Additionally, DFT studies also shed light on the adsorption structure of HDPy+/ReO 4 − and the origin of adsorption selectivity. Moreover, four adsorption-desorption cycles suggest that the HDPy-bent has good durability and reusability. Furthermore, ReO 4 − can be removed completely and recovered fractionally by using the chromatography column packed with HDPy-bent from simulated groundwater samples. The work presented herein demonstrates a low-cost adsorbent which can efficiently remove 99Tc from contaminated water. [ABSTRACT FROM AUTHOR]

• 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]

99Tc primarily exists high mobility in the natural aqueous environment due to its extremely high solubility and non-complexing features, which can easily cause radioactive pollution. We herein report a general strategy for constructing a novel resin (SiPAN-PEI) with multiple positive charges nitrogen, exhibiting ultrafast adsorption kinetics (< 3 min), superior adsorption capacities (463.96 mg g−1), and excellent selectivity in the presence of excess competitive anions, which exceed those of most commercial resins. Moreover, based on impressive structure stability in extreme conditions, SiPAN-PEI can still maintain superior adsorption abilities after suffering irradiation, calcination, and immersion in strong acid. In addition, the separation performance kept excellently after five loading-washing-eluting cycles and the total adsorption ratio can still reach 97 %. Outstandingly, SiPAN-PEI can remove most of ReO 4 - from simulated nuclear wastewater through a sequential injection automatic separation system and can reduce the concentration of ReO 4 - to the maximum concentration standard set by the World Health Organization (WHO) in a short time. Leveraging density functional theory calculations and other characteristics clearly elucidated adsorption mechanism of anion-exchange between Cl- and TcO 4 -/ReO 4 -. In terms of superior adsorption property, SiPAN-PEI is demonstrated to be a pretty candidate for 99Tc elimination from wastewater. [Display omitted] • A novel resin SiPAN-PEI was successfully synthesized for selective capture of 99Tc. • SiPAN-PEI exhibited excellent adsorption ability of 99Tc in harsh conditions. • Multiple positive charge nitrogen plays a critical role in capture of 99Tc. • SiPAN-PEI demonstrated efficiency capture of 99Tc in simulated wastewater. [ABSTRACT FROM AUTHOR]