Spatial Engineering Direct Cooperativity between Binding Sites for Uranium Sequestration.
Spatial Engineering Direct Cooperativity between Binding Sites for Uranium Sequestration.
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DOI:
10.1002/advs.202001573
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发表时间:
2021-01
期刊:
影响因子:
--
通讯作者:
Ma S
中科院分区:
文献类型:
--
作者:
Sun Q;Song Y;Aguila B;Ivanov AS;Bryantsev VS;Ma S
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. The affinity of a specific chelating group in sorbent materials toward analyte of interest is significantly increased through engineering their spatial distribution, at an appropriate arrangement, driving the cooperative binding and thereby improved performance.
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