With rising atmospheric CO2 levels, increasing share of renewable energy and advancing carbon
capture technologies are essential to mitigate climate change. Adsorption-based separation using
solid adsorbents is a promising approach for various carbon capture applications. However, several
materials challenges remain regarding their capacity, selectivity, stability, etc. Comprehensive
experimental characterization of adsorbents is crucial to advance their development for targeted
CO2 capture applications. This project focused on using different experimental techniques for
assessing adsorbent performance, with an emphasis on measuring competitive CO2/H2O
adsorption equilibria of both reference and novel adsorbents. A laboratory bench-top
breakthrough analyser was designed and constructed to enable binary adsorption measurements
using small sample quantities under industrially relevant conditions. Commercial activated carbon
(AC) and zeolite 13X (MS13X) were characterized as benchmark adsorbents, establishing a useful
reference point for novel adsorbent materials such as Metal Organic Frameworks (MOFs). An
experimental exploration into the functionalization of MOFs to improve their CO2 adsorption
performance was also undertaken. MIL-100(Fe) was synthesized via sol-gel synthesis using n-butylamine as a modulating ligand forming a powder and a monolith, both materials underwent
thorough evaluation across various performance metrics. The monolithic form, with its structured
morphology, showed promise by overcoming the pressure drop limitations of the powder form
and doubling its volumetric CO2 adsorption capacity. However, these novel functionalized
materials did not surpass the overall adsorbent performance of benchmark materials when
considering additional metrics such as kinetics, selectivity, etc. The complete materials
characterization and assessment framework developed and applied herein can help identify optimal
novel adsorbents based on targeted industrial conditions. Overall, this thesis advanced
experimental techniques for adsorbent evaluation by constructing a novel adsorption analyser and
provided guidance on best practices for multicomponent adsorption measurement. These results
showcase the importance of collaborative, integrated research efforts to accelerate the scale-up of
adsorption-based carbon capture processes.