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Structural Characterization of Gas A...
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Plonka, Anna Monika.
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Structural Characterization of Gas Adsorption in Metal Organic Frameworks.
紀錄類型:
書目-電子資源 : Monograph/item
正題名/作者:
Structural Characterization of Gas Adsorption in Metal Organic Frameworks./
作者:
Plonka, Anna Monika.
出版者:
Ann Arbor : ProQuest Dissertations & Theses, : 2015,
面頁冊數:
231 p.
附註:
Source: Dissertation Abstracts International, Volume: 76-11(E), Section: B.
Contained By:
Dissertation Abstracts International76-11B(E).
標題:
Mineralogy. -
電子資源:
http://pqdd.sinica.edu.tw/twdaoapp/servlet/advanced?query=3712826
ISBN:
9781321898941
Structural Characterization of Gas Adsorption in Metal Organic Frameworks.
Plonka, Anna Monika.
Structural Characterization of Gas Adsorption in Metal Organic Frameworks.
- Ann Arbor : ProQuest Dissertations & Theses, 2015 - 231 p.
Source: Dissertation Abstracts International, Volume: 76-11(E), Section: B.
Thesis (Ph.D.)--State University of New York at Stony Brook, 2015.
This item is not available from ProQuest Dissertations & Theses.
Selective adsorption and sequestration of carbon dioxide from sources of anthropogenic emissions is important to mitigate the growing level of the atmospheric CO2. Solid state adsorbents, such as metal organic frameworks (MOFs), are proposed as an alternative to the currently used toxic and corrosive alkanolamine solutions. The aim of this work was to understand the interactions between adsorbed gases and a pore surface of crystalline MOFs at a molecular level, and identify the connection between geometry and gas selectivity.
ISBN: 9781321898941Subjects--Topical Terms:
516743
Mineralogy.
Structural Characterization of Gas Adsorption in Metal Organic Frameworks.
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Selective adsorption and sequestration of carbon dioxide from sources of anthropogenic emissions is important to mitigate the growing level of the atmospheric CO2. Solid state adsorbents, such as metal organic frameworks (MOFs), are proposed as an alternative to the currently used toxic and corrosive alkanolamine solutions. The aim of this work was to understand the interactions between adsorbed gases and a pore surface of crystalline MOFs at a molecular level, and identify the connection between geometry and gas selectivity.
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In contrast to current trends in the design of MOFs, we described the unique mechanism responsible for a high CO2/N2 adsorption selectivity in a Ca-based MOF: Ca(sdb), (sdb: 4,4'-sulfonyldibenzoate), even in the presence of water in the gas stream. Single crystal XRD experiments of gas-loaded samples revealed that the v-shaped linker provides a "pi-pocket" formed by two phenyl rings, and that CO2 locate between the rings, resulting in a high heat of adsorption. To determine the gas adsorption performance in situ in the presence of water, we used X-ray Diffraction (XRD) simultaneously with differential scanning calorimetry (XRD-DSC). The XRD-DSC technique allows measurements of heat flow that provide enthalpy of adsorption, while at the same time XRD allows evaluation of structural responses during MOF activation and gas adsorption. We also used XRD-DSC to determine the performance of Cd(sdb), the Cd-based analogue of Ca(sdb): Cd(sdb) shows a high selectivity for CO2 over N2. In situ vacuum-swing XRD-DSC allowed us to determine the heat of adsorption values of the adsorbate; results of these studies were consistent with the pi--CO2 interaction as the origin of the selectivity.
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The newly described "pi-pocket" is a potential site for a selective adsorption of gases other than CO2. Hydrocarbon gases (C2Hn), such as ethane, ethylene and acetylene, were adsorbed on Ca(sdb) and on another Ca-based MOF: Ca(tcpb) [tcpb: 1,2,4,5-tetrakis(4-carboxyphenyl)benzene] with a high measured energy of interaction. Structural data suggest that C 2Hn interact with the organic linkers within the MOF frameworks through C-H···pi and C-H··· O interactions. The knowledge acquired here can promote systematic synthetic searches for novel materials that can serve as selective solid-state adsorbents.
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Finally, the formation of Ca-based Metal Organic Frameworks was studied using different structural isomers of pyridinedicarboxylic acid. Nine MOF materials were synthesized and structurally analyzed. The atomic arrangements in the crystal structure of resultant MOFs are based on a variety of the inorganic structural motifs, ranging from isolated polyhedra to infinite chains, a layer or a 3-D connectivity, depending on the linker geometry and the synthetic condition.
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