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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]

Technetium-99m (99mTc) is an important medical radionuclide. Due to the crisis in supply of molybdenum-99 (99Mo), production of 99mTc directly via the 100Mo (p, 2 n) reaction by cyclotron was proposed. In this process, the most critical challenge is to rapidly and efficiently separate 99mTc from high concentration of molybdenum. In this work, a novel ligand, bis(N,N -dibutyldiglycolamide)dibenzo-18-crown-6 (BisDBDGA-DB18C6) was successfully synthesized and used for extraction of TcO 4 - /ReO 4 - from molybdenum. The results demonstrated that BisDBDGA-DB18C6 expressed excellent selectivity for TcO 4 - with a high separation factor of 1.6 × 105 against Mo, a fast extraction kinetic (within 45 s), and a high extraction capacity of 211 mmol ReO 4 - (99TcO 4 -)/per mole of extractant. The extraction mechanism was proposed as a co-interaction of macrocyclic crown ether and N,N -dibutyldiglycolamide group through slope analysis, FT-IR, ESI-MS, 1H NMR titration and theory calculations. Importantly, 99Tc in the organic phase can be quantitatively (> 99%) and easily back-extracted using deionized water, which can be directly used for medical applications. [Display omitted] • A novel ligand BisDBDGA-DB18C6 was first prepared. • The tailored BisDBDGA-DB18C6 exhibits ultrafast extraction kinetic (within 45 s). • Superior extraction performance toward Tc/Re over Mo is confirmed and evaluated. • The solution is stripped with deionized water for direct medical applications. [ABSTRACT FROM AUTHOR]