Drinking water contaminated with arsenic is a worldwide problem, especially in developing nations. The research presented in this dissertation describes two major goals: development of hybrid homopolymer polyacrylonitrile (PAN)-based sorbents for arsenate removal from drinking water and understanding regeneration of arsenate from ferric hydroxide-based adsorbents. The homopolymer PAN fiber was chemically modified to introduce functional groups using NaOH and hydrazine hydrate (HH) separately, or in combination of both. The modified fibers were characterized using Fourier transform infrared spectroscopy (FTIR) and ion exchange measurements. The ferric hydroxides were impregnated onto functionalized fibers using two iron loading procedures. The best arsenate removal performance was obtained using the simplest pretreatment procedure of soaking in 10% NaOH at 95 °C for ninety min, followed by precipitation coating of ferric hydroxide. This suggests that adsorbents based on a low-cost PAN fabric may be produced in developing areas of the world where commercial products may not be available. A density functional theory (DFT) molecular modeling was used to compare free energies of reactions and activation barriers in the formation of arsenate-ferric hydroxide complexes. Slow kinetics associated with arsenate adsorption and desorption attributed to the high activation barriers in forming and breaking bonds with the ferric hydroxides. Another aspect of regeneration study focused on the effects of underlying properties of the ferric hydroxides-loaded adsorbents on arsenate recovery. The arsenate loaded ferric hydroxide adsorbent containing no or weak base functionalities can be regenerated using NaOH, while addition of NaCl to NaOH solution is required for same recovery of arsenate from the adsorbents containing strong base anion exchange functionalities. Moreover, the irreversible fraction of arsenate on the adsorbent can be reduced by increasing the concentration of NaOH. Thus, understanding arsenate desorption kinetics and effects of support properties of ferric hydroxide-based adsorbents are important for environmental fate of arsenate and in designing adsorption systems for removing arsenate from potable water.
| Identifer | oai:union.ndltd.org:arizona.edu/oai:arizona.openrepository.com:10150/337308 |
| Date | January 2014 |
| Creators | Chaudhary, Binod K. |
| Contributors | Farrell, James, Farrell, James, Arnold, Bob, Reyes, Sierra, Chorover, Jon |
| Publisher | The University of Arizona. |
| Source Sets | University of Arizona |
| Language | en_US |
| Detected Language | English |
| Type | text, Electronic Dissertation |
| Rights | Copyright © is held by the author. Digital access to this material is made possible by the University Libraries, University of Arizona. Further transmission, reproduction or presentation (such as public display or performance) of protected items is prohibited except with permission of the author. |
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