Proceedings of nanoGe Fall Meeting19 (NFM19)
DOI: https://doi.org/10.29363/nanoge.nfm.2019.223
Publication date: 18th July 2019
Catalytic CO2 conversion to chemical feedstocks and carbon-based fuels powered by renewable energy sources constitutes a promising approach towards achieving a closed carbon cycle. Advancing this technology in the future relies strongly on optimization of the present catalytic systems to drive the conversion reaction with minimal energy losses and precise selectivity. In this respect, molecular catalytic centers as well as electrocatalytically-active 2D framework materials heterogenized onto suitable conductive support materials have emerged as interesting catalytic systems with prospective application potentials. The rational improvement such systems is based on the availability of in-depth information on the catalytic reaction mechanism that would allow for precise fine-tuning of the catalytic properties via chemical variations. To this end, particularly vibrational spectroelectrochemistry has established as a valuable tool to reveal and monitor the complex reactions. In contrast to other spectroscopic methods, this technique can be readily employed under in situ (aqueous) conditions and derives directly data on the catalytic steps at a molecular level.
This presentation discusses the versatility of (surface-enhanced) vibrational spectroelectrochemistry to study CO2 reduction catalysis specifically promoted by highly-active heterogenized molecular transition metal complexes and phthalocyanine-based 2D framework materials. The examples from the latest research include the application of operando IR absorption and confocal (resonance) Raman spectroscopy coupled to electrochemical control revealing crucial information on the reaction mechanism of the heterogenized catalysts with relevant implications on their afforded reactivity and selectivity.[1,2] The presentation concludes with an assessment of future prospects and novel experimental designs to increase the wealth of information that operando vibrational spectro-electrochemistry can derive.