Publication date: 15th December 2025
Increasing global energy demands have led to a rapid rise in environmental concerns, largely driven by the growing CO2 levels in the atmosphere. Inspired by photosynthesis in nature, photocatalytic materials have gained significant attention as a method of producing value-added chemicals using CO2 as feedstock material, mitigating the escalating greenhouse effect.
Owing to their high surface area, stability and tuneability, porous materials such as Metal Organic Frameworks (MOFs) and Covalent Organic Frameworks (COFs) are promising candidates for photocatalysis. Despite this, the absence of catalytically active metal sites and poor stabilities have hindered COFs and MOFs respectively. In addition, in terms of photocatalysis, MOFs and COFs have faced limitations due to factors including insufficient light absorption capabilities and quenching processes.[1,2] These problems could be addressed by introducing metal complexes into stable COF backbones, forming porous Metalloligand Covalent Organic Frameworks (MLCOFs), as demonstrated by Han et al., who used a Ru-MLCOF to photocatalytically produce syngas from CO2.[3,4]
However, a better understanding of the atomic structure of MLCOFs is expected to improve their performance and design. Due to the low crystallinity of these frameworks, obtaining a complete structural understanding of MLCOFs is a challenge. Nevertheless, using a theoretical and experimental approach, MLCOFs can be fully characterised, as illustrated in a Ru(tpy)2-based MLCOF.[5] Taking inspiration from this, we have synthesised a novel MLCOF, instead using Fe(tpy)2 metalloligands and tetrasubstituted pyrene nodes. With the aim of producing a more environmentally friendly alternative, we use iron, an earth abundant transition metal. Morphological changes in response to the modulation of monomer ratios, shifting from globular to coral-like will be presented. In addition, the use of a freeze-thaw processing step, further shifts the morphology to stacked elongated sheet-like structures. A complete structural characterisation has been conducted, including crystallographic investigations using 3D electron diffraction and X-ray diffraction techniques. Prelimianry CO2 reduction tests have been carried out and the results will be presented.
Funding support from the Irish Research Council (GOIPG/2025/889)
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