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Engineering novel porous materials for carbon capture and storage

Al-Janabi, Nadeen

[Thesis]. Manchester, UK: The University of Manchester; 2017.

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Abstract

Global warming along with the climate change derived from the World's demand for energy are among the greatest challenges to our society. To tackle climate change issue, research must focus on proposing practical approaches for carbon emissions reduction and environmental remediation.This thesis focuses on carbon dioxide separation mainly from flue gases (major sources of carbon dioxide emissions) using metal organic frameworks (MOFs) to reduce its impact on the global warming hence the climate change. MOFs are a class of crystalline porous adsorbents with structures that attract CO2 selectively and store it in their porous frameworks.Over the course of this PhD research, the fundamental aspects of these materials, as well as their practical applications, have been investigated. For example, the synthesis recipe of copper (II) benzene-1,3,5-tricarboxylate (CuBTC) MOF was improved to deliver a product of high yield (> 89%) and free of by-product. Also, a mechanism study on the hydrothermal stability CuBTC MOF was carried out under simulated flue gas conditions and delivered the first experimental proof of the decomposition mechanism of CuBTC MOF caused by the water vapour. The fundamental understanding of the stability of materials then motivated the research into the development of a facile method of using an economic functional dopant (i.e. glycine) to strengthen the structure of CuBTC MOF (completely stable towards water vapour), as well as to improve the selectivity of resulting materials to CO2 (by 15% in comparison to the original CuBTC MOF). The suitability of the CuBTC MOF for fixed bed adsorption processes was also assessed using a combined experimental and process simulation method.In addition to the experimental approaches, molecular simulation based on grand canonical Monte Carlo method was also used to understand the effect of structural defects of MOFs on the CO2 adsorption isotherms.