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Title: Polyamidoxime chain length drives emergent metal-binding phenomena

Abstract

Emergence is complex behavior arising from the interactions of many simple constituents that do not display such behavior independently. Here, polyamidoxime (PAO) uranium adsorbents show such phenomena, as recent works articulate that the polymer binds uranium differently than the monomeric constituents. In order to investigate the origins of this emergent uranium-binding behavior, we synthesized a series of amidoxime polymers with low polydispersity and small molecules with lengths ranging from 1 to 125 repeat units. Following immersion in a uranyl-containing solution, the local, intermediate, and macroscopic structures were investigated by X-ray absorption fine structure (XAFS) spectroscopy, small angle neutron scattering (SANS), and dynamic light scattering (DLS). Fits of the extended XAFS (EXAFS) region revealed a progressive change in uranium coordination environment as a function of polymer molecular weight, identifying chain length as a driving force in emergent metal binding and resolving the controversy over how amidoxime adsorbents bind uranium.

Authors:
ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1]
  1. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1542249
Alternate Identifier(s):
OSTI ID: 1476369
Grant/Contract Number:  
AC05-00OR22725
Resource Type:
Accepted Manuscript
Journal Name:
Physical Chemistry Chemical Physics. PCCP (Print)
Additional Journal Information:
Journal Name: Physical Chemistry Chemical Physics. PCCP (Print); Journal Volume: 21; Journal Issue: 2; Journal ID: ISSN 1463-9076
Publisher:
Royal Society of Chemistry
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 36 MATERIALS SCIENCE

Citation Formats

Earl, Lyndsey D., Do, Changwoo, Wang, Yangyang, and Abney, Carter W. Polyamidoxime chain length drives emergent metal-binding phenomena. United States: N. p., 2018. Web. doi:10.1039/c8cp02198h.
Earl, Lyndsey D., Do, Changwoo, Wang, Yangyang, & Abney, Carter W. Polyamidoxime chain length drives emergent metal-binding phenomena. United States. doi:10.1039/c8cp02198h.
Earl, Lyndsey D., Do, Changwoo, Wang, Yangyang, and Abney, Carter W. Thu . "Polyamidoxime chain length drives emergent metal-binding phenomena". United States. doi:10.1039/c8cp02198h.
@article{osti_1542249,
title = {Polyamidoxime chain length drives emergent metal-binding phenomena},
author = {Earl, Lyndsey D. and Do, Changwoo and Wang, Yangyang and Abney, Carter W.},
abstractNote = {Emergence is complex behavior arising from the interactions of many simple constituents that do not display such behavior independently. Here, polyamidoxime (PAO) uranium adsorbents show such phenomena, as recent works articulate that the polymer binds uranium differently than the monomeric constituents. In order to investigate the origins of this emergent uranium-binding behavior, we synthesized a series of amidoxime polymers with low polydispersity and small molecules with lengths ranging from 1 to 125 repeat units. Following immersion in a uranyl-containing solution, the local, intermediate, and macroscopic structures were investigated by X-ray absorption fine structure (XAFS) spectroscopy, small angle neutron scattering (SANS), and dynamic light scattering (DLS). Fits of the extended XAFS (EXAFS) region revealed a progressive change in uranium coordination environment as a function of polymer molecular weight, identifying chain length as a driving force in emergent metal binding and resolving the controversy over how amidoxime adsorbents bind uranium.},
doi = {10.1039/c8cp02198h},
journal = {Physical Chemistry Chemical Physics. PCCP (Print)},
number = 2,
volume = 21,
place = {United States},
year = {2018},
month = {9}
}

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Works referenced in this record:

Preparation of hydrophilic amidoxime fibers by cografting acrylonitrile and methacrylic acid from an optimized monomer composition
journal, October 2000

  • Kawai, Tomomi; Saito, Kyoichi; Sugita, Kazuyuki
  • Radiation Physics and Chemistry, Vol. 59, Issue 4, p. 405-411
  • DOI: 10.1016/S0969-806X(00)00298-X