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Synthesis and Design Cationic Metal-...

Colinas, Ian R.

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Synthesis and Design Cationic Metal-Organic Frameworks for Perchlorate Remediation and Bactericidal Applications.

紀錄類型:	書目-電子資源 : Monograph/item
正題名/作者:	Synthesis and Design Cationic Metal-Organic Frameworks for Perchlorate Remediation and Bactericidal Applications./
作者:	Colinas, Ian R.
出版者:	Ann Arbor : ProQuest Dissertations & Theses, : 2018,
面頁冊數:	170 p.
附註:	Source: Dissertation Abstracts International, Volume: 80-03(E), Section: B.
Contained By:	Dissertation Abstracts International80-03B(E).
標題:	Chemistry. -
電子資源:	http://pqdd.sinica.edu.tw/twdaoapp/servlet/advanced?query=10828048
ISBN:	9780438534193

Synthesis and Design Cationic Metal-Organic Frameworks for Perchlorate Remediation and Bactericidal Applications.
Colinas, Ian R.

Synthesis and Design Cationic Metal-Organic Frameworks for Perchlorate Remediation and Bactericidal Applications. - Ann Arbor : ProQuest Dissertations & Theses, 2018 - 170 p.

Source: Dissertation Abstracts International, Volume: 80-03(E), Section: B.

Thesis (Ph.D.)--University of California, Santa Cruz, 2018.

The issue of perchlorate (ClO4-) as an emerging pollutant has gained significant attention globally as it has been detected in groundwater, surface water, soils, and crops of many countries including the United States, Japan, China, India, Korea, and Germany. The toxic effects of this anionic pollutant result from the disruption of the thyroid gland, which is blocked and inhibited from iodide uptake due to the slightly larger ionic radii of perchlorate. Such impairment of the thyroid gland can occur upon exposure to parts per billion (ppb) perchlorate levels, and it has been associated with detrimental development effects in fetuses and children. Most perchlorate is manufactured for its use as a primary ingredient in solid rocket propellants in both military and aerospace technology, and its widespread occurrence in the environment has resulted from its improper disposal and high mobility in aqueous environments.

ISBN: 9780438534193Subjects--Topical Terms:

516420
Chemistry.

Synthesis and Design Cationic Metal-Organic Frameworks for Perchlorate Remediation and Bactericidal Applications.
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500 $a Source: Dissertation Abstracts International, Volume: 80-03(E), Section: B.
500 $a Adviser: Scott R.J. Oliver.
502 $a Thesis (Ph.D.)--University of California, Santa Cruz, 2018.
520 $a The issue of perchlorate (ClO4-) as an emerging pollutant has gained significant attention globally as it has been detected in groundwater, surface water, soils, and crops of many countries including the United States, Japan, China, India, Korea, and Germany. The toxic effects of this anionic pollutant result from the disruption of the thyroid gland, which is blocked and inhibited from iodide uptake due to the slightly larger ionic radii of perchlorate. Such impairment of the thyroid gland can occur upon exposure to parts per billion (ppb) perchlorate levels, and it has been associated with detrimental development effects in fetuses and children. Most perchlorate is manufactured for its use as a primary ingredient in solid rocket propellants in both military and aerospace technology, and its widespread occurrence in the environment has resulted from its improper disposal and high mobility in aqueous environments.
520 $a Currently, anion exchange resins are the standard material used for perchlorate remediation. These consist of inexpensive polymeric matrices with limited chemical and thermal stability due to their organic nature. In addition, their performance is severely affected by their poor selectivity towards perchlorate and lack of recyclability. Therefore, high performance anion exchangers that can efficiently capture perchlorate are sought. Extended inorganic crystalline materials are promising candidates for the replacement of organic resins due to their higher stability but these materials are often neutral or anionic, thus extended cationic structures are of special interest in the field of anion separation. Layered double hydroxides (LDHs) are cationic isostructural clay-like materials that have been widely studied for their anion exchanging properties. However, LDHs are known to have a high affinity towards ubiquitous carbonate ions, as well as tendency to re-intercalate water molecules immediately after calcination. This drastically decreases their overall uptake capacity and selectivity for the capture of anionic pollutants from wastewater.
520 $a Metal-organic frameworks are promising materials in the field of separation due to the tunability in their structure and function. Cationic metal-organic frameworks are a subclass of these crystalline extended materials, which can be easily prepared by introducing neutral organic ligands for cationic metals and weakly coordinating anions that balance the overall cationic charge of the framework. These cationic materials offer a viable alternative to conventional anion exchangers due to their robust tunable frameworks that can exchange anions reversibly at high adsorption capacities.
520 $a A detailed methodology for the efficient separation of perchlorate from water was demonstrated by utilizing a cationic MOF consisting of three-dimensional [Ag-bipy]+ chains arranged in a T-shaped pattern with nitrate anions counter-balancing the framework. Ambient conditions were used for both the synthesis of this cationic material, silver 4,4'- bipyridine nitrate (SBN), as well as the exchange resulting in the formation silver 4,4'- bipyridine perchlorate (SBP). The exchange was complete within 90 minutes and the capacity was 354 mg of ClO4-/g of SBN, representing 99% ClO4- removal. SBN exhibited superior performance compared to that of current anion exchangers such as the resins Amberlite IRA-400 (249 mg/g) and Purolite A530E (104 mg/g), as well as layered double hydroxides (28 mg/g). Unlike resins and layered double hydroxides, SBN could be successfully regenerated in nitrate solution at 70 °C with new crystal formation, allowing indefinite cycling for perchlorate capture.
520 $a An in-depth investigation of the host-guest interaction of cationic [Ag-bipy] + MOFs with perchlorate was carefully performed. The structural transformation and flexibility of SBN upon formation of SBP was evaluated by monitoring the anion exchange dynamics using a combination of powder X-ray diffraction (PXRD) with multinuclear 13C, 15N and 109Ag solid-state nuclear magnetic resonance (NMR) spectra at different time intervals of the anion exchange. The structural transformation from SBN to SBP is complete within 70 minutes and was determined to take place by a solvent-mediated process. This pathway is confirmed by the morphological changes of the two crystalline materials observed by scanning electron microscopy (SEM). The understanding of such structural dynamics highlighted in this study provides crucial insights for the rational design of related MOFs toward the selective capture of environmental pollutant oxo-anions. (Abstract shortened by ProQuest.).
590 $a School code: 0036.
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650 4 $a Inorganic chemistry. $3 3173556
650 4 $a Organic chemistry. $3 523952
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