Spatial Engineering Direct Cooperativity between Binding Sites for Uranium Sequestration
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.
- Authors:
-
[4]
- Univ. of South Florida, Tampa, FL (United States). Dept. of Chemistry
- Univ. of North Texas, Denton, TX (United States). Dept. of Chemistry
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Chemical Sciences Division
- Univ. of South Florida, Tampa, FL (United States). Dept. of Chemistry; Univ. of North Texas, Denton, TX (United States). Dept. of Chemistry
- Publication Date:
- Research Org.:
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Nuclear Physics (NP); Robert A. Welch Foundation; National Science Foundation (NSF)
- OSTI Identifier:
- 1787559
- Alternate Identifier(s):
- OSTI ID: 1841483
- Grant/Contract Number:
- NE0008281; B‐0027; CBET-1706025; AC05-00OR22725
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Advanced Science
- Additional Journal Information:
- Journal Volume: 8; Journal Issue: 2; Journal ID: ISSN 2198-3844
- Publisher:
- Wiley
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 73 NUCLEAR PHYSICS AND RADIATION PHYSICS; cooperative binding; environmental remediation; porous organic frameworks; radionuclide sequestration; uranium recovery
Citation Formats
Sun, Qi, Song, Yanpei, Aguila, Briana, Ivanov, Aleksandr S., Bryantsev, Vyacheslav S., and Ma, Shengqian. Spatial Engineering Direct Cooperativity between Binding Sites for Uranium Sequestration. United States: N. p., 2020.
Web. doi:10.1002/advs.202001573.
Sun, Qi, Song, Yanpei, Aguila, Briana, Ivanov, Aleksandr S., Bryantsev, Vyacheslav S., & Ma, Shengqian. Spatial Engineering Direct Cooperativity between Binding Sites for Uranium Sequestration. United States. https://doi.org/10.1002/advs.202001573
Sun, Qi, Song, Yanpei, Aguila, Briana, Ivanov, Aleksandr S., Bryantsev, Vyacheslav S., and Ma, Shengqian. Fri .
"Spatial Engineering Direct Cooperativity between Binding Sites for Uranium Sequestration". United States. https://doi.org/10.1002/advs.202001573. https://www.osti.gov/servlets/purl/1787559.
@article{osti_1787559,
title = {Spatial Engineering Direct Cooperativity between Binding Sites for Uranium Sequestration},
author = {Sun, Qi and Song, Yanpei and Aguila, Briana and Ivanov, Aleksandr S. and Bryantsev, Vyacheslav S. and Ma, Shengqian},
abstractNote = {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.},
doi = {10.1002/advs.202001573},
journal = {Advanced Science},
number = 2,
volume = 8,
place = {United States},
year = {Fri Dec 04 00:00:00 EST 2020},
month = {Fri Dec 04 00:00:00 EST 2020}
}
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