Publication date: 6th November 2020
DMC is a valuable chemical used on industrial scale for both production (e.g. carbonylation reactions) and in end products (e.g. paints and batteries). DMC is currently formed by thermal catalysis but can be formed electrocatalytically, it is a carbonylation product of methanol1, formed electrochemically by the reaction 2CH3OH + CO à (CH3O)2CO + 2H+ + 2e-.
The purpose of the work is to understand the fundamental aspects of the carbonylation reaction over an electrode surface, i.e. by heterogeneous electrocatalysis, rather than homogeneous or indirection electrosynthesis. Knowing the steps of formation and the reaction intermediates involved will allow us to develop the catalytic system in a rational manner as well as apply the knowledge to later reactions of interest (e.g. carbonylation of other alcohols, such as phenol, to form valuable products). Understanding the active site and mechanism of the reaction is paramount for rational optimisation strategies.
Different transition metals (Cu, Au, Pt) have been tested for their activity towards DMC production1,2,3. Au is more active than Pd in terms of current efficiency as well as current density (Figure 1), whereas Cu catalysis DMC synthesis via an inefficient solution phase mechanism. We have used different techniques to understand catalyst activity: in situ infrared spectroelectrochemistry (in situ FTIR) and headspace gas chromatography mass spectrometry (HS-GC-MS). The results that we have obtained so far have been discussed in combination with a theoretical analysis which has helped us understand the mechanisms involved. Further development is underway for optimising the catalyst as well as reactor system.
[1] Šarić, M., Davies, B.J.V. et al, Green Chem., 2019, 21, 6200-6209
[2] Davies, B.J.V. et al, ACS Catal., 2019, 9, 2, 859-866
[3] Davies, B.J.V. et al, J. Phys. Chem. C, 2019, 123, 20, 12762-12772
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