Atmospheric CO2 Capture and Conversion

Aims The aim of the project is to use simple inorganic systems to selectively capture atmospheric CO2 and convert it to the carbonate anion for use in a series of functional inorganic materials. The mechanism and catalytic activity of the capture and conversion of CO2 will be investigated looking at metal and ligand type, solvent, anion and electronic effects in an effort to maximize the systems potential. The resultant inorganic materials will be investigated in terms of their physical and electronic properties. Finally the conversion of these materials to calcium or magnesium carbonate will be studied in the context of long-term carbon storage solutions. Introduction A report by the Committee on Climate Change has recently announced that to meet the goals of the Paris climate change agreement in reducing domestic emissions to net zero, the UK must set out a strategy to develop new technology to remove anthropogenic carbon dioxide (CO2).

1 The aviation and farming industries are unlikely to become carbon neutral so to achieve the target of an overall net zero domestic emission, CO2 will
need to be removed directly from the atmosphere. A pragmatic approach to this problem involves carbon capture and sequestration (CCS) technology at large sources such as coal power plants. However this is not only a significant technical challenge but a costly one; between 25-40% of the energy usage of the plant would be on the CCS technology alone.2 A more attractive approach would be to capture CO2 directly from the atmosphere and then recycle it into a variety of useful chemicals or feedstocks.3 This is challenging when you consider the relative lack of reactivity of CO2, the low concentration of CO2 in the atmosphere and the requirement of a system that can selectively target CO2 and convert it into useful functional materials. A recent study4 of ours has shown exactly that; a porous network containing cores of carbonate anions which could only have come from atmospheric CO2. This offers a remarkable model system to investigate the mechanism of the selective capture and conversion of atmospheric CO2 and subsequent recycling into chemically and industrially useful functional materials. This process has added utility in that it is water friendly and cheap metal sources such as iron and copper could be used offering real long-term possibilities in terms of upscaling, manufacturing and green credentials. Characterisation and supervisory team. Year one – This will involve exploratory synthesis of a library of lanthanide and transition metal complexes containing targeted polypryidyl ligands with the synthetic aspects characterised by a battery of characterisation techniques including mass spectrometry, NMR, UV-Vis, FTIR, thermogravimetric analysis, differential scanning calorimetry and single crystal Xray crystallography.

Year two – This will involve an investigation of the mechanism of the CO2 uptake and conversion potential of these materials in a range of
CO2 environments. Year three – The physical properties and ability of these materials to be converted to simple metal carbonates such as calcium carbonate will be investigated. The single crystal X-ray crystallography will be undertaken at the UK National Crystallography Service at Southampton and all other measurements be performed within PABS and via existing collaborations. Any prospective PhD student will become an expert in inorganic synthesis and characterisation and be first author on a string of high quality publications at the time of their PhD completion. The supervisor team consists of Dr Ian A Gass and Dr Peter Cragg with relevant expertise in chemical synthesis and inorganic characterisation. 1. “UK Climate Action following the Paris Agreement”, Committee on Climate Change, Report October 2016. 2. D. M. Allesandro, B. Smit and J. R. Long, Carbon Dioxide Capture: Prospects for New Materials, Angew. Chem. Int. Ed., 2010, 49, 6058-6082. 3. J. Kothandaraman,