Publication date: 10th April 2024
The industrial production of ethylene (C2H4) is central to modern societal applications such as plastics, epoxides and synthetic rubber. However, the commercial process involving the steam cracking of ethane/naphtha is the second-biggest CO2-generating process in industry.1 Thus, novel synthesis routes are necessary to decarbonize industrial C2H4 production. In 1982, Keller and Bhasin first reported on an alternative C2H4 production method, the oxidative coupling of methane (OCM),2 which can directly convert CH4 into C2H4. Unfortunately, this OCM approach is limited by significant “deep oxidation” where CH4 is instead combusted to CO/CO2 and H2O. To improve the C2 (C2H4 and C2H6) selectivity and yield of OCM, recent works have integrated OCM activity into solid oxide electrolyzers. In this electrochemical OCM (EOCM) approach, O2− ions from the cathode are transported to the anode where they oxidise CH4 to yield the desired C2 products. While the initial results are promising,3 little is known about the fundamental surface chemistry which contributes to the selective CH4 to C2H4 conversion in these systems.
In order to study the mechanistic details of selective CH4 activation, herein we use La0.3Sr0.7TiO3 as a mixed ionic-electronic conducting anode for EOCM. Combined electrochemical and gas chromatographic analyses demonstrate that this anode can successfully yield the desired C2 products and can respond to changes in the O2− flux. In particular, we illustrate that the C2 selectivity can be tuned using the applied potential: we show an unprecedented tuneability in the C2 selectivity with enhancements of >3x at higher current densities relative to values obtained at lower current densities. These increases in the C2 selectivity are then correlated with the onset of oxygen evolution at the anode surface. Thus, we hypothesize that by coupling CH4 activation to the oxygen evolution reaction, it is possible to selectively produce the active oxygen species which are necessary for selective CH4 activation towards the C2 products. These results furnish an understanding of how to increase both the CH4 conversion and C2 selectivity and have finally broken the inverse relationship between the CH4 conversion and the C2 selectivity that has traditionally limited thermochemical OCM approaches.
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