This thesis presents a combination of material synthesis and characterization with process modeling. In it, the CO2 adsorption properties of hydrotalcites are enhanced through the production of novel supported hybrids (carbon nanotubes and graphene oxide) and the promotion with alkali metals. Hydrogen is regarded as a sustainable energy carrier, since the end users produce no carbon emissions. However, given that most of the hydrogen produced worldwide comes from fossil fuels, its potential as a carbon-free alternative depends on the ability to capture the carbon dioxide released during manufacture. Sorption-enhanced hydrogen production, in which CO2 is removed as it is formed, can make a major contribution to achieving this. The challenge is to find solid adsorbents with sufficient CO2 capacity that can work in the right temperature window over repeated adsorption-desorption cycles.

Nominated as an outstanding Ph.D. thesis by Imperial College London, UK

Introduction.- Literature Review.- Experimental Methods.- Layered Double Hydroxides Supported on Multi-Walled Carbon Nanotubes.- Layered Double Hydroxides Supported on Graphene Oxide for CO2 Adsorption.- Influence of Alkali Metals on Layered Double Hydroxides Supported on Graphene Oxide for CO2 Adsorption.- CO2 Adsorption on Unsupported and Graphene Oxide Supported Layered Double Hydroxides in a Fixed-Bed.- Sorption-Enhanced Methanol-to-Shift for H2 Production: Thermodynamics and Catalyst Selection.- Conclusions and Future Work.