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Synthesis and gas sorption study of microporous metal-organic frameworks for hydrogen and methane storage
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Title
Synthesis and gas sorption study of microporous metal-organic frameworks for hydrogen and methane storage
Identifier
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http://hdl.rutgers.edu/1782.2/rucore10001600001.ETD.16719
Identifier
ETD_553
Language
LanguageTerm
(authority = ISO 639-3:2007)
English
Genre
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theses
Subject
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Topic
Chemistry and Chemical Biology
Subject
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(authority = ETD-LCSH)
Topic
Hydrogen--Storage
Subject
(ID = SBJ-1);
(authority = ETD-LCSH)
Topic
Methane--Storage
Abstract
One of the strategic goals of seeking for renewable energy sources/carriers that are clean and abundant is to replace fossil fuel with alternative fuel such as hydrogen gas. The U.S. Department of Energy has set forth specific cost and performance targets for utilizing hydrogen and natural gas for commercial purpose. In this study, a series of porous [M(L)(P)0.5] materials (where, M2+=Zn, Co, Ni, Cu; L (or linker) = obba, bdc, ndc; P (or pillar) = bpy or ted) were synthesizes via solvothermal reactions and evaluated on their ability of hydrogen and methane storage. By incorporating L groups with different length, microporous metal-organic framework (MOF) structures having controlled pore sizes were constructed. Single crystal X-ray diffraction study showed that they possess up to 60 % free space and the diameters of the pores are in the range of 3.5 ?? ~ 9 ??. The tunable and permanent porosity and gas storage capacity of these materials were explored by low and high pressure sorption study. At low pressure high resolution argon sorption experiments revealed that these MOF materials have very high surface area, up to 3282 m2/g. The hydrogen sorption study showed that reversible hydrogen adsorption/desorption can be achieved with pore size larger than 6 ??. From the high pressure hydrogen study, a 5.48 wt% of hydrogen uptake was achieved at 77 K and ~60 bar on [Ni(ndc)(ted)0.5], and 36 g/L of high volumetric density was also observed for [Zn(bdc)(ted)0.5] at the same temperature and ~40 bar. The interaction between hydrogen and MOF materials was analyzed in terms of isosteric heat of adsorption. Generally, a range of 5.0 ~ 7.5 kJ/mol of heat of adsorption energy was found for the structures investigated. These findings suggest that physisorption is the primary force of hydrogen adsorption on the internal surface of MOF materials. Crystals of [Zn(bdc)(ted)0.5] exhibit high methane storage capability at 298 K, as well as separation capability between hydrogen and methane gas, as several other selected MOF materials.
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xvii, 141 pages
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Ph.D.
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Includes bibliographical references.
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Lee
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JeongYong
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JeongYong Lee
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Li
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Jing
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Jing Li
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Hall
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Eugene
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Eugene Hall
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Warmuth
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Ralf
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Ralf Warmuth
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Rutgers University
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Graduate School - New Brunswick
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2007
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2007
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Graduate School - New Brunswick Electronic Theses and Dissertations
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rucore19991600001
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doi:10.7282/T3JH3MKF
Genre
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ETD doctoral
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Rights
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The author owns the copyright to this work.
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Copyright protected
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Open
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JeongYong Lee
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Rutgers University. Graduate School - New Brunswick
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Non-exclusive ETD license
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Author Agreement License
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I hereby grant to the Rutgers University Libraries and to my school the non-exclusive right to archive, reproduce and distribute my thesis or dissertation, in whole or in part, and/or my abstract, in whole or in part, in and from an electronic format, subject to the release date subsequently stipulated in this submittal form and approved by my school. I represent and stipulate that the thesis or dissertation and its abstract are my original work, that they do not infringe or violate any rights of others, and that I make these grants as the sole owner of the rights to my thesis or dissertation and its abstract. I represent that I have obtained written permissions, when necessary, from the owner(s) of each third party copyrighted matter to be included in my thesis or dissertation and will supply copies of such upon request by my school. I acknowledge that RU ETD and my school will not distribute my thesis or dissertation or its abstract if, in their reasonable judgment, they believe all such rights have not been secured. I acknowledge that I retain ownership rights to the copyright of my work. I also retain the right to use all or part of this thesis or dissertation in future works, such as articles or books.
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