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Dendritic Anion Hosts: Perchlorate Uptake by G5-NH_2 Poly(propyleneimine) Dendrimer in Water and Model Electrolyte Solutions

Diallo, Mamadou S. and Falconer, Kwesi and Johnson, James H., Jr. and Goddard, William A., III (2007) Dendritic Anion Hosts: Perchlorate Uptake by G5-NH_2 Poly(propyleneimine) Dendrimer in Water and Model Electrolyte Solutions. Environmental Science and Technology, 41 (18). pp. 6521-6527. ISSN 0013-936X. doi:10.1021/es0710959. https://resolver.caltech.edu/CaltechAUTHORS:20170426-090124312

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Abstract

Perchlorate (ClO_4^-) has emerged as a major groundwater and surface water contaminant in the United States. Ion exchange (IX) is the most widely used technology for treating water containing lower concentrations of perchlorate (<100 ppb). However, a major drawback of IX is the need for frequent regeneration or disposal of the perchlorate-laden resins. As a first step toward the development of high-capacity, selective and recyclable dendritic ligands for the recovery of perchlorate from aqueous solutions by dendrimer filtration, we tested the hypothesis that dendrimers with hydrophobic cavities and positively charged internal groups should selectively bind ClO_4^- over more hydrophilic anions such as Cl^-, NO_3^-, SO_4^(2-), and HCO_3^-. We measured the uptake of ClO_4^- by the fifth generation (G5-NH_2) poly(propyleneimine) (PPI) dendrimer with a diaminobutane core and terminal NH_2 groups in deonized water and model electrolyte solutions as a function of (i) anion−dendrimer loading, (ii) solution pH, (iii) background electrolyte concentration, and (iv) reaction time. The ClO_4^- binding capacity of this dendrimer is comparable to those of perchlorate-selective IX resins. However, its ClO_4^- binding kinetics is faster and reaches equilibrium in ∼1 h. Note also that only a high pH (∼9.0) aqueous solution is needed to release more than 90% of the bound ClO_4^- anions by deprotonation of the dendrimer tertiary amine groups. The overall results of this study suggest that dendritic macromolecules such as the G5-PPI NH_2 dendrimer provide ideal building blocks for the development of high-capacity, selective and recyclable ligands for the recovery of anions such as perchlorate from aqueous solutions by dendrimer enhanced filtration.


Item Type:Article
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URLURL TypeDescription
http://dx.doi.org/10.1021/es0710959DOIArticle
http://pubs.acs.org/doi/abs/10.1021/es0710959PublisherArticle
http://pubs.acs.org/doi/suppl/10.1021/es0710959PublisherSupporting Information
ORCID:
AuthorORCID
Diallo, Mamadou S.0000-0002-2571-1568
Goddard, William A., III0000-0003-0097-5716
Additional Information:© 2007 American Chemical Society. Received 26 October 2006. Date accepted 29 May 2007. Published online 11 August 2007. Published in print 1 September 2007. 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. Funding for this work was provided by the National Science Foundation (NIRT CBET Award # 0506951). Supplemental funding for this research was provided to Howard University by the Department of Energy (DOE Massie Chair Grant DE-FG02-94EW11423). We thank Prof. Charles Glass and Ms. Lily Wan of the Department of Civil Engineering at Howard University for their assistance with the ion chromatography analyses.
Funders:
Funding AgencyGrant Number
NSFCBET-0506951
Department of Energy (DOE)DE-FG02-94EW11423
Issue or Number:18
DOI:10.1021/es0710959
Record Number:CaltechAUTHORS:20170426-090124312
Persistent URL:https://resolver.caltech.edu/CaltechAUTHORS:20170426-090124312
Official Citation:Dendritic Anion Hosts:  Perchlorate Uptake by G5-NH2 Poly(propyleneimine) Dendrimer in Water and Model Electrolyte Solutions Mamadou S. Diallo, Kwesi Falconer, James H. Johnson, Jr., and William A. Goddard, III Environmental Science & Technology 2007 41 (18), 6521-6527 DOI: 10.1021/es0710959
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:76941
Collection:CaltechAUTHORS
Deposited By: Ruth Sustaita
Deposited On:26 Apr 2017 17:30
Last Modified:15 Nov 2021 17:04

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