Electroreduction of carbon dioxide to formate at high current densities using tin and tin oxide gas diffusion electrodes

Abstract

We investigate tin (Sn) and tin oxide (SnO2) nanoparticle catalysts deposited on gas diffusion layers for the electrochemical reduction of carbon dioxide (CO2) to formate. The performance and durability of these electrodes was evaluated in a gas-fed electrolysis cell with a flowing liquid electrolyte stream and an integrated reference electrode. The SnO2 electrodes achieved peak current densities of 385 ± 19 mA cm−2 while the Sn electrodes achieved peak current densities of 214 ± 6 mA cm−2, both at a formate selectivity > 70%. The associated peak formate production rates of 7.4 ± 0.6 mmol m−2 s−1 (Sn) and 14.9 ± 0.8 mmol m−2 s−1 (SnO2) were demonstrated for a 1-h electrolysis and compare favorably to prior literature. Post-test analyses reveal chemical and physical changes to both cathodes during electrolysis including oxide reduction at applied potentials more negative than − 0.6 V versus RHE, nanoparticle aggregation, and catalyst layer erosion. Understanding and mitigating these decay processes is key to extending electrode lifetime without sacrificing formate generation rates or process efficiency.

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Acknowledgements

This work availed the MRSEC Shared Experimental Facilities at MIT, supported by the National Science Foundation under award number DMR-1419807. The authors acknowledge the financial support of DOE SBIR Contract #DE-SC0015173. The authors thank Michael Orella of the Brushett Research Group for insightful discussions and assistance with experiments.

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Sen, S., Brown, S.M., Leonard, M. et al. Electroreduction of carbon dioxide to formate at high current densities using tin and tin oxide gas diffusion electrodes. J Appl Electrochem 49, 917–928 (2019). https://doi.org/10.1007/s10800-019-01332-z

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Keywords

  • Electrochemical reduction
  • Carbon dioxide
  • Gas diffusion electrode
  • Flow electrolyzer
  • Formate production
  • Tin oxide