Polyamidoxime chain length drives emergent metal-binding phenomena

Earl, Lyndsey D.; Do, Changwoo; Wang, Yangyang; Abney, Carter W.

doi:10.1039/c8cp02198h

Title: Polyamidoxime chain length drives emergent metal-binding phenomena

Journal Article · 26 September 2018 · Physical Chemistry Chemical Physics. PCCP

DOI: https://doi.org/10.1039/c8cp02198h · OSTI ID:1542249

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Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)

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.

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Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 1542249

Alternate ID(s):: OSTI ID: 1476369

Journal Information:: Physical Chemistry Chemical Physics. PCCP, Journal Name: Physical Chemistry Chemical Physics. PCCP Journal Issue: 2 Vol. 21; ISSN 1463-9076; ISSN PPCPFQ

Publisher:: Royal Society of ChemistryCopyright Statement

Country of Publication:: United States

Language:: English

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