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Co-electrolysis of CO2 and glycerol as a pathway to carbon chemicals with improved technoeconomics due to low electricity consumption

Abstract

The renewable electricity-driven electroreduction of carbon dioxide (CO2) offers an alternative pathway to producing carbon chemicals that are traditionally manufactured using fossil fuels. Typical CO2 electroreduction approaches couple cathodic CO2 reduction with the anodic oxygen evolution reaction (OER), resulting in approximately 90% of the electricity input being consumed by the OER. Here, we explore alternatives to the OER and show that the anodic electro-oxidation of glycerol (a byproduct of industrial biodiesel and soap production) can lower electricity consumption by up to 53%. This reduces the process’s operating costs and carbon footprint, thus opening avenues for a carbon-neutral cradle-to-gate process even when driven by grid electricity (~13% renewables today), as well as economical production of the 12-electron products ethylene and ethanol. This study may thus serve as a framework for the design of CO2 electroreduction processes with low electricity requirements, enhancing their CO2 utilization potential and economic viability.

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Fig. 1: Overview of select CO2 electroreduction products, along with the current industrial methods to manufacture these products.
Fig. 2: Scope of the cradle-to-gate CO2 emissions analysis, and description of the steps involved in the industrial implementation of CO2 electroreduction.
Fig. 3: Optimizing separation parameters for the purification of CO2 electroreduction products.
Fig. 4: Electrochemical performance for the electroreduction of CO2 to CO on silver, coupled to O2 evolution, glycerol electro-oxidation or glucose electro-oxidation at the anode.
Fig. 5: Electrochemical performances for the electroreduction of CO2 to HCOO on tin, and to C2H4 and C2H5OH on copper, coupled to O2 evolution or glycerol electro-oxidation at the anode.

Data availability

The electrochemical data that support the plots, as well other findings of this study, are available in the Supplementary Information.

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Acknowledgements

The authors acknowledge financial support from the International Institute for Carbon Neutral Energy Research (WPI-I2CNER), sponsored by the Japanese Ministry of Education, Culture, Sports, Science and Technology, as well as the Dow Chemical Company, and Glenn E. and Barbara R. Ullyot for graduate fellowships to S.V. The 1H NMR experiments were performed in the School of Chemical Sciences NMR Laboratory at the University of Illinois.

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Authors and Affiliations

Authors

Contributions

S.V. conceived the project, performed the cradle-to-gate CO2 analysis, designed and conducted the electrochemical experiments, analysed the data and wrote the manuscript. S.L. prepared the electrodes, contributed to the electrochemical experiments and commented on the manuscript. P.J.A.K. conceived the project, directed the research and wrote the manuscript.

Corresponding author

Correspondence to Paul J. A. Kenis.

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Competing interests

The authors have filed a patent application (US patent application number 15/971,223) on technology related to the processes described in this article.

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Supplementary information

Supplementary Information

Supplementary Figs. 1–3, Supplementary Tables 1–11, Supplementary references

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Verma, S., Lu, S. & Kenis, P.J.A. Co-electrolysis of CO2 and glycerol as a pathway to carbon chemicals with improved technoeconomics due to low electricity consumption. Nat Energy 4, 466–474 (2019). https://doi.org/10.1038/s41560-019-0374-6

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