4.8 Article

Highly selective plasma-activated copper catalysts for carbon dioxide reduction to ethylene

Journal

NATURE COMMUNICATIONS
Volume 7, Issue -, Pages -

Publisher

NATURE PUBLISHING GROUP
DOI: 10.1038/ncomms12123

Keywords

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Funding

  1. German Federal Ministry of Education and Research (Bundesministerium fur Bildung und Forschung, BMBF) [03SF0523 - 'CO2EKAT']
  2. Cluster of Excellence RESOLV at RUB - Deutsche Forschungsgemeinschaft [EXC 1069]
  3. US National Science Foundation [NSF-Chemistry 1213182, NSF-DMR 1207065, NSF CHE 1534630]
  4. Office of Basic Energy Sciences of the US Department of Energy [DE-FG02-08ER15995, DE-FG02-03ER15476]
  5. U.S. DOE [DE-SC0012653]
  6. U.S. DOE Office of Science Facility [DE-SC0012704]
  7. UT Austin
  8. Office of Science, Office of Basic Energy Sciences, of the U.S. Department of Energy [DE-AC02-05CH11231]
  9. U.S. Department of Energy (DOE) [DE-SC0012653] Funding Source: U.S. Department of Energy (DOE)
  10. Direct For Mathematical & Physical Scien
  11. Division Of Materials Research [1207065] Funding Source: National Science Foundation
  12. Division Of Chemistry
  13. Direct For Mathematical & Physical Scien [1213182] Funding Source: National Science Foundation
  14. Division Of Chemistry
  15. Direct For Mathematical & Physical Scien [1534630] Funding Source: National Science Foundation

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There is an urgent need to develop technologies that use renewable energy to convert waste products such as carbon dioxide into hydrocarbon fuels. Carbon dioxide can be electrochemically reduced to hydrocarbons over copper catalysts, although higher efficiency is required. We have developed oxidized copper catalysts displaying lower overpotentials for carbon dioxide electroreduction and record selectivity towards ethylene (60%) through facile and tunable plasma treatments. Herein we provide insight into the improved performance of these catalysts by combining electrochemical measurements with microscopic and spectroscopic characterization techniques. Operando X-ray absorption spectroscopy and cross-sectional scanning transmission electron microscopy show that copper oxides are surprisingly resistant to reduction and copper(+) species remain on the surface during the reaction. Our results demonstrate that the roughness of oxide-derived copper catalysts plays only a partial role in determining the catalytic performance, while the presence of copper(+) is key for lowering the onset potential and enhancing ethylene selectivity.

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