Carbon dioxide capture using metal-organic frameworks (MOFs) : a thesis presented in partial fulfilment of the requirements of the degree of Doctor of Philosophy in Chemistry at Massey University, Manawatu, New Zealand. EMBARGOED until further notice.

Abstract

Modern life and industrial processes without efficient CO₂ capture are increasingly unsustainable. Achieving high CO₂ uptake, selectivity over other gases, and efficient regeneration is critical for carbon capture technologies. Adsorbent-based systems offer the potential to separate CO₂ with high capacity and selectivity under mild regeneration conditions. However, low CO₂ concentrations, the presence of impurities and water vapor in flue gas, and the dynamic nature of industrial capture make effective large-scale separation challenging. In this thesis, MUF-16, a metal-organic framework (MOF), was characterized and demonstrated for CO₂ capture in real-world applications. We bridge the gap between laboratory-scale experiments and large-scale implementation through a combination of experimental and simulation methods. Molecular, numerical, and computational models at both small and large scales were developed to describe and predict the static and dynamic properties of MUF-16, ensuring its feasibility under a wide range of real-world conditions. These models were validated against experimental data to ensure reliable predictions. Furthermore, a multivariate (MTV) approach was employed, both theoretically and experimentally, to enhance CO₂ capture performance by synthesizing analogues of MUF-16. This work establishes a platform that highlights the key initial steps and considerations required when commercializing an adsorbent and introducing it into large-scale applications. The results of this thesis demonstrate that MUF-16 is an excellent adsorbent, capable of selectively capturing CO₂ with high performance under various conditions. These attributes highlight its strong potential to become a commercially viable material for CO₂ capture.