DOI: https://doi.org/10.29363/nanoge.ecat.2023.019
Publication date: 10th October 2023
The electrochemical reduction of CO2 is a valuable strategy to convert this gas into value-added, carbon-containing chemicals. C1 products, such as carbon monoxide (CO), formaldehyde (HCHO) or methanol (CH3OH) can find applications in the industry or as fuels, but their economic value is limited. C2 or C3 products, such as ethylene (C2H4) or propylene (C3H6), are used in such high amounts in the industry (millions of tons per year), that their production from CO2 feedstocks is key to valorizing this gas.
The electrocatalytic reduction of CO2 suffers from one major drawback: the selectivity towards a given product. Decades of research on catalyst development have only been able to achieve high selectivity towards CO or formic acid (HCOOH). Amongst catalysts, transition metal macrocycles have emerged as economical, robust, and effective catalysts for the electroreduction of CO2. Unfortunately, they can only reduce CO2 into C1 products such as CO [1] or methanol [2]. The formation of C2+ products upon electroreduction of CO2 have only been observed, up to now, for copper catalysts.
We have found that a commercially available molecular macrocycle, iron phthalocyanine, is able to convert CO2 into small quantities of methane (CH4), but also C2, C3 and C4 products. Control experiments show that both CO2 and the catalyst are required to observe these products. Gas chromatography and mass spectrometry were used, together with 13C labelled CO2 substrate, to demonstrate the origin of the carbon atoms in the products. X-ray absorption spectroscopy performed under operating conditions confirmed the molecular nature of the catalyst throughout the experiment. Catalytic experiments were performed with alternate substrates, which allowed us to propose a mechanistic hypothesis for this reaction.
We are grateful to the Agence National de la Recherche (Grant n°ANR-18-CE05-0007) for a young researcher grant to B.L.-K. and a PhD fellowship to S.-T.D.
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