Decoupled electrochemistry allows for the separation of a traditional electrochemical step from th ecatlaytic step of a reaction. Using redox mediators instead of electrodes to drive the target the reaction, the electrochemistry becomes dependnet on an efficient reduction reaction that can be opposite someting less kinetically challenging than convention. This means lower overpotentials, which in turn means less electricity is applied.
The catalytic process is then driven by the charged redox mediators, but in a setting away from th e lectrode. Electolysis without the electrodes! This has been demonstrated for water splitting in numerous conditions (since Kathryn's early work in 2011 at EPFL with Prof. Hubert Girault). However, realising the reduction of an additional species, especially one as challenging as CO2, was new. We have realised these reactions since 2020.
The catalysts being studied on this project are bimetallic materials and two-dimensional MXenes, as well as copper materials as a bench mark for performance. The key is to identify materials that will encourage CO2 reduction while limiting hydrogen evolution. So far we have had great success with engineered bismuth nanoparticles and PVA-coated gold.
Redox mediators generated on this project are similar to the range of catholyte solutions used in redox flow batteries. The reducing capability of the mediator dictates the driving force of the reaction. however, we are increasingly seeing that what governs conventional electrochemical eletron transfer is not necessarily the same in decoupled systems...
A robust and reliable analytical set up to quantify CO2 reduction products is critical to evaluating and developing new catalytic materials and optimising reactor designs. This project will develop techniques using relatively new appraoches; Gas chromatography with a Barrier Ionisation Discharge detector and Online Electrochemical Mass Spectrometry.
Members of the project went to Lyon this Septmeber to present on their work conceerning CO2 reduction. A total of 3 posters were presented over the course of the conference, covering all aspects of the project. Sam presented on his MXenes as CO2 catalysts, Daniel overviewed the highs and lows of using electrochemical mass spectrometry as a tool for product analysis and Mark presented on our recent proof of concept data showing CO2 reduction using redox mediator solutions!
Members of the project went to Manchester in September 2024 to present on their work concerning CO2 reduction. Kathryn delivered a Keynote lecture on Decoupled CO2 Reduction, Mark Potter gave a talk on the spcifics of CO2 reduction to formate, Dr Hamza Annath presented a poster of Zn MOFS with copper doping for CO2 reduction to CO. In a related work Dr Luis Pinho gave a presentation the decoupled hydrogen reduction reaction using non platinum group catalysts. We also had a poster presented on redox targeting flow batteries from Brian Lewis.
Kathryn and Mark attended Electrochem 2024 held at a former monastry in Raitenhaslach on the border of Germany and Austria. In the beautiful autumn sun we heard a wide range of talks on complex electrochemical systems. The meeting was followed on with the Redox Shields workshop, part of the legacy of Prof. Nicolas Plumere's ERC funding. some ecellent foundational electrochemistry was presented. Kathryn and Mark gave talks on allthings redox flow nad decoupled electrochem.
Kathryn had the honour of delivering one of the five conference plenary lectures to a broad energy storage audience in Edinburgh for the UKES 26. The work introduced electrochemical energy storage and the hybrid storage opportunities of decoupled electrochemistry. the audience was very diverse but it was a fantastic conference looking at all electricity and thermal energy storage strategies.
Kathryn had the honour of delivering one of the four conference Keynote lectures to an audience of over 300 delegates. The work outlined all our progress with decoupled electrochemistry since Kathryn's inaugural work in 2014. The rest of the group also gave talks, including decoupled CO2 reduction by Cr mediators from Mark, All iron flow batteries from Eduardo and Redox targeting flow batteries using monomer-polymer chemistry.