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首页> 外文期刊>Environmental Science & Technology: ES&T >Modulating Anion Nanotraps via Halogenation for High-Efficiency ~(99)TcO_4~-/ReO_4~-Removal under Wide-Ranging pH Conditions
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Modulating Anion Nanotraps via Halogenation for High-Efficiency ~(99)TcO_4~-/ReO_4~-Removal under Wide-Ranging pH Conditions

机译:Modulating Anion Nanotraps via Halogenation for High-Efficiency ~(99)TcO_4~-/ReO_4~-Removal under Wide-Ranging pH Conditions

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摘要

Efficient and sustainable methods for ~(99)TcO4~-removal from acidic nuclear waste streams,contaminated water,and highly alkaline tank wastes are highly sought after.Herein,we demonstrate that ionic covalent organic polymers(iCOPs)possessing imidazolium-N~+ nanotraps allow the selective adsorption of ~(99)TcO4~-under wide-ranging pH conditions.In particular,we show that the binding affinity of the cationic nanotraps toward ~(99)TcO4~-can be modulated by tuning the local environment around the nanotraps through a halogenation strategy,thereby enabling universal pH ~(99)TcO4~-removal.A parent iCOP-1 possessing imidazolium-N~+ nanotraps showed fast kinetics(reaching adsorption equilibrium in 1 min),a high adsorption capacity(up to 1434.1 ± 24.6 mg/g),and exceptional selectivity for ~(99)TcO4_ and ReO_4~-(nonradioactive analogue of ~(99)TcO4~)removal in contaminated water.By introducing F groups near the imidazolium-N~+ nanotrap sites(iCOP-2),a ReO_4~-removal efficiency over 58% was achieved in 60 min in 3 M HNO3 solution.Further,introduction of larger Br groups near the imidazolium-N~+ binding sites(iCOP-3)imparted a pronounced steric effect,resulting in exceptional adsorption performance for ~(99)TcO4~-under super alkaline conditions and from low-activity waste streams at US legacy Hanford nuclear sites.The halogenation strategy reported herein guides the task-specific design of functional adsorbents for ~(99)TcO4~-removal and other applications.

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