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Dendritic Chelating Agents. 2. U(VI) Binding to Poly(amidoamine) and Poly(propyleneimine) Dendrimers in Aqueous Solutions

Diallo, Mamadou S. and Arasho, Wondwossen and Johnson, James H. and Goddard, William A., III (2008) Dendritic Chelating Agents. 2. U(VI) Binding to Poly(amidoamine) and Poly(propyleneimine) Dendrimers in Aqueous Solutions. Environmental Science and Technology, 42 (5). pp. 1572-1579. ISSN 0013-936X. https://resolver.caltech.edu/CaltechAUTHORS:20170315-090949812

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Abstract

Chelating agents are widely employed in many separation processes used to recover uranyl [U(VI)] from contaminated aqueous solutions. This article describes an experimental investigation of the binding of U(VI) to poly(amidoamine) [PAMAM] and poly(propyleneimine) [PPI] dendrimers in aqueous solutions. We combine fluorescence spectroscopy with bench scale ultrafiltration experiments to measure the extent of binding and fractional binding of U(VI) in aqueous solutions of these dendrimers as a function of (i) metal−ion dendrimer loading, (ii) dendrimer generation, (iii) dendrimer core and terminal group chemistry, and (iv) solution pH and competing ligands (NO_3^−, PO_4^(3−), CO_3^(2−), and Cl^−). The overall results of this study suggest that uranyl binding to PAMAM and PPI dendrimers in aqueous solutions involves the coordination of the UO22+ ions with the dendrimer amine, amide, and carboxylic groups. We find significant binding of U(VI) to PAMAM dendrimers in (i) acidic solutions containing up to 1.0 M HNO_3 and H_3PO_4 and (ii) in basic solutions containing up to 0.5 M Na_2CO_3. However, no binding of U(VI) by PAMAM dendrimers is observed in aqueous solutions containing 1.0 M NaCl at pH 3.0. These results strongly suggest that PAMAM and PPI dendrimers can serve as high capacity and selective chelating ligands for U(VI) in aqueous solutions.


Item Type:Article
Related URLs:
URLURL TypeDescription
http://dx.doi.org/10.1021/es0715905DOIArticle
http://pubs.acs.org/doi/abs/10.1021/es0715905PublisherArticle
http://pubs.acs.org/doi/suppl/10.1021/es0715905PublisherSupporting Information
ORCID:
AuthorORCID
Goddard, William A., III0000-0003-0097-5716
Additional Information:© 2008 American Chemical Society. Received June 28, 2007. Revised manuscript received October 22, 2007. Accepted October 29, 2007. Publication Date (Web): January 23, 2008. This work was carried out in the Materials Process Simulation Center of the Division of Chemistry and Chemical Engineering at the California Institute of Technology and in the Department of Civil Engineering at Howard University. The data collected in this study provided background information for two provisional patent applications on the development of dendrimer based chelating agents and separation systems for recovering actinides from aqueous solutions. Funding for this work was provided by the National Science Foundation (NIRT CBET Award no. 050695) (Caltech) and the Department of Energy (DOE Massie Chair Grant DE-FG02-94EW11423 (Howard University).
Funders:
Funding AgencyGrant Number
NSFCBET-050695
Department of Energy (DOE)DE-FG02-94EW11423
Issue or Number:5
Record Number:CaltechAUTHORS:20170315-090949812
Persistent URL:https://resolver.caltech.edu/CaltechAUTHORS:20170315-090949812
Official Citation:Dendritic Chelating Agents. 2. U(VI) Binding to Poly(amidoamine) and Poly(propyleneimine) Dendrimers in Aqueous Solutions Mamadou S. Diallo, Wondwossen Arasho, James H. Johnson, Jr., and William A. Goddard III Environmental Science & Technology 2008 42 (5), 1572-1579 DOI: 10.1021/es0715905
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:75135
Collection:CaltechAUTHORS
Deposited By: Tony Diaz
Deposited On:15 Mar 2017 18:28
Last Modified:03 Oct 2019 16:47

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