Carbon dioxide conversion is rapidly gaining attention as CO2 is increasingly being regarded as a feedstock (as opposed to a waste product) for the preparation of a wide range of value added commodities, such as useful chemical raw materials or energy rich products. However, an efficient CO2 transformation process is challenging, but it has great potential for the demand of future resources that do not rely on petrochemical sources. The reduction reaction of CO2 requires high-yield, an input of energy and a catalyst. Therefore, if a renewable carbon-free primary energy source is used to power the CO2 reduction, such a process may lead to the use of waste CO2 as a renewable raw material. Among various experimental techniques, ElectroCatalytic Reduction (ECR) has promise as it can convert electrical energy into chemicals (energy storage). This well known electrochemically-driven reaction can be performed on pure or composite metal electrocatalysts, but it requires large overpotentials, electrode poisoning often occurs and selectivity is generally poor. These problems can be addressed using molecular catalysts. In the past thirty years several transition metal complexes, able to convert CO2 by ECR, have been studied. This includes systems based on Re, Ru and Os bipyridyl carbonyl systems. However very few earth abundant metal based molecular electro-catalysts have been reported so far. Much of our current work is focussed on developing and studying new Mn molecular catalysts and understanding their CO2 reducing catalytic properties via the ECR pathway, in order to gain a better understanding of their mechanisms, all with the aim of improving and advancing the field of CO2 valorisation. This work follows closely on from some of our recent results involving selective ECR of CO2. Here we will present our ongoing research which is helping to better understand ligand effects on the CO2 catalytic reduction process; especially the important role that ligands can have on catalytic mechanisms and therefore efficiency, product selectivity, yield and overall catalyst stability under electro-catalytic conditions.

Electrocatalytic conversion of CO2 using molecular manganese carbonyl based catalysts

253rd National Meeting (2017)

The official archive and repository for all ACS Meetings & Expositions abstracts and select posters or presentations.