Topics in Catalysis

, Volume 58, Issue 1, pp 57–66 | Cite as

Integration of Anodic and Cathodic Catalysts of Earth-Abundant Materials for Efficient, Scalable CO2 Reduction

  • Rishi Parajuli
  • James B. Gerken
  • Kunttal Keyshar
  • Ian Sullivan
  • Narayanappa Sivasankar
  • Kyle Teamey
  • Shannon S. Stahl
  • Emily Barton Cole
Original Paper

Abstract

A fully integrated electrochemical cell for co-production of formate (HCOO) and oxygen (O2) from carbon dioxide (CO2) and water using only earth-abundant elements has been developed. The process converts CO2 to formate using electrons derived from anodic water oxidation. A novel cathodic catalyst system, consisting of a tin (Sn) cathode in combination with the soluble heterocycle 2-picoline, was identified for CO2 reduction. Water oxidation takes place at a fluorine-doped tin oxide electrode coated with an electrodeposited cobalt oxide (CoOx) electrocatalyst. Use of 2-picoline as a soluble cathodic co-catalyst lowered the overpotential and enhanced the stability of the Sn-mediated CO2 reduction process. Fluorophosphate served as a redox-stable electrolyte to buffer the anode compartment at mildly acidic pH (~ 5 to 5.5), thereby stabilizing the CoOx electrocatalyst and supporting efficient water oxidation. The complete electrochemical cell maintained a stable cell voltage of less than 3 V over 5 days, with an average formate faradaic yield of 34 %. These results are presented together with an economical analysis of large-scale solar-driven production of formate/formic acid from CO2 and water.

Keywords

Water oxidation CO2 electroreduction Electrocatalyst Formic acid Cobalt oxide Tin 

Notes

Acknowledgments

The authors would like to thank Dr. Charles G. Fry for advice on NMR measurements, Dr. Liliana Lopez Aguilar for assistance with IC-MS analysis, and George Leonard for assistance with GC analysis. Research conducted in the Stahl lab was partially supported by an NSF CCI Grant CHE-0802907 and by NMR facility support under NSF Grant CHE-9629688.

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Copyright information

© Springer Science+Business Media New York 2014

Authors and Affiliations

  • Rishi Parajuli
    • 1
  • James B. Gerken
    • 2
  • Kunttal Keyshar
    • 1
    • 3
  • Ian Sullivan
    • 1
    • 4
  • Narayanappa Sivasankar
    • 1
  • Kyle Teamey
    • 1
  • Shannon S. Stahl
    • 2
  • Emily Barton Cole
    • 1
  1. 1.Liquid LightMonmouth JunctionUSA
  2. 2.Department of ChemistryUniversity of Wisconsin-MadisonMadisonUSA
  3. 3.Department of Mechanical Engineering & Materials ScienceRice UniversityHoustonUSA
  4. 4.Department of ChemistryNorth Carolina State UniversityRaleighUSA

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