Journal
SMALL
Volume 16, Issue 24, Pages -Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/smll.202001896
Keywords
CO2 reduction; electrocatalysis; flue gas; gas phase electrolysis; single-atom catalysts
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Funding
- National Key R&D Program of China [2016YFB0600901]
- National Natural Science Foundation of China [21773124]
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Single-atom Co catalyst Co-Tpy-C with well-defined sites is synthesized by pyrolysis of a Co terpyridine (Tpy) organometallic complex. The Co-Tpy-C catalyst exhibits excellent activity for the electrochemical CO2 reduction reaction in aqueous electrolyte, with CO faradaic efficiency (FE) of over 95% from -0.7 to -1.0 V (vs RHE). By comparison, catalysts without Co or Tpy ligand added do not show any high CO FE. When simulated flue gas with 15% of CO2 is used as the source of CO2, CO FE is kept at 90.1% at -0.5 V versus RHE. During gas phase flow electrolysis using simulated flue gas, the CO partial current density is further increased to 86.4 mA cm(-2) and CO FE reached >90% at the cell voltage of 3.4 V. Experiments and density functional theory calculations indicate that uniform single-atom Co-N-4 sites mainly contribute to the high activity for CO2 reduction.
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