Qi Sun1, Yanpei Song2, Briana Aguila1, Aleksandr S Ivanov3, Vyacheslav S Bryantsev3, Shengqian Ma1,2. 1. Department of Chemistry University of South Florida 4202 E. Fowler Avenue Tampa FL 33620 USA. 2. Department of Chemistry University of North Texas 1508 W Mulberry St Denton TX 76201 USA. 3. Chemical Sciences Division Oak Ridge National Laboratory P. O. Box 2008 Oak Ridge TN 37831 USA.
Abstract
Preorganization is a basic design principle used by nature that allows for synergistic pathways to be expressed. Herein, a full account of the conceptual and experimental development from randomly distributed functionalities to a convergent arrangement that facilitates cooperative binding is given, thus conferring exceptional affinity toward the analyte of interest. The resulting material with chelating groups populated adjacently in a spatially locked manner displays up to two orders of magnitude improvement compared to a random and isolated manner using uranium sequestration as a model application. This adsorbent shows exceptional extraction efficiencies, capable of reducing the uranium concentration from 5 ppm to less than 1 ppb within 10 min, even though the system is permeated with high concentrations of competing ions. The efficiency is further supported by its ability to extract uranium from seawater with an uptake capability of 5.01 mg g-1, placing it among the highest-capacity seawater uranium extraction materials described to date. The concept presented here uncovers a new paradigm in the design of efficient sorbent materials by manipulating the spatial distribution to amplify the cooperation of functions.
Preorganization is a basic design principle used by nature that allows for synergistic pathways to be expressed. Herein, a full account of the conceptual and experimental development from randomly distributed functionalities to a convergent arrangement that facilitates cooperative binding is given, thus conferring exceptional affinity toward the analyte of interest. The resulting material with chelating groups populated adjacently in a spatially locked manner displays up to two orders of magnitude improvement compared to a random and isolated manner using class="Chemical">uranium sequestratioclass="Chemical">n as a model applicatioclass="Chemical">n. This adsorbeclass="Chemical">nt shows exceptioclass="Chemical">nal extractioclass="Chemical">n efficieclass="Chemical">ncies, capable of reduciclass="Chemical">ng the class="Chemical">n class="Chemical">uranium concentration from 5 ppm to less than 1 ppb within 10 min, even though the system is permeated with high concentrations of competing ions. The efficiency is further supported by its ability to extract uranium from seawater with an uptake capability of 5.01 mg g-1, placing it among the highest-capacity seawateruranium extraction materials described to date. The concept presented here uncovers a new paradigm in the design of efficient sorbent materials by manipulating the spatial distribution to amplify the cooperation of functions.
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