Nickel-Modified Bifunctional MOF-on-MOF Systems for Upgrading Sequestered CO2

Objective

The increasing climate crisis demands urgent advancements in carbon capture and conversion (CCC) technologies to mitigate rising atmospheric CO2 levels. Current methods face critical limitations, including high energy demands, poor performance under realistic conditions, and a lack of integration between CO2 capture and catalytic advancement. This project, Nickel-Modified Bifunctional MOF-on-MOF Systems for Upgrading Sequestered CO2 (NIMBUS), aims to overcome current limitations by taking advantage of the remarkable properties of metal-organic frameworks (MOFs), such as their porosity, outstanding mechanical stability, chemical versatility, and reactivity. The strategy involves the rational design of a novel MOF-on-MOF core-shell architecture, by synergistically combining three widely single-optimized approaches: (1) enhanced CO2 uptake through metal doping and defect-functionalisation, (2) humidity resistance via a hydrophobic shell, and (3) catalytic conversion to valuable-added products using embedded Ni nanoparticles. Thanks to the integrations of these functionalities into a single material, NIMBUS aims to achieve a significant increase in CO2 adsorption and selectivity for CH₄ production under industrial flue gas conditions (60% RH, 40–120°C). The project employs advanced characterization techniques, including synchrotron-based analysis to establish structure-property relationships and optimize material performance, enabling the rational design of robust CCC materials. By combining defect-functionalisation, metal doping, and core-shell assembly, NIMBUS aims to create a sustainable pathway toward a circular carbon economy, aligning with global climate goals by converting CO2 from a waste product into a renewable resource.