Journal
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 60, Issue 51, Pages 26582-26586Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202113135
Keywords
adsorption strength; carbon dioxide electroreduction; key reaction intermediates; single-atom catalysis; temperature dependence
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Funding
- National Natural Science Foundation of China [22125205, 92045302]
- Dalian National Laboratory for Clean Energy [DNL201924, DNL202007]
- Dalian Institute of Chemical Physics [DICP DMTO201702]
- Strategic Priority Research Program of the Chinese Academy of Sciences [XDB17020200]
- CAS Youth Innovation Promotion [Y201938]
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In this study, the temperature-dependent CO2 reduction reactions over Fe-N-C and Ni-N-C single-atom catalysts were investigated, revealing variations in selectivity and activity. The differences in CO Faradaic efficiency and current density between Fe-N-C and Ni-N-C catalysts at different temperatures were found to be attributed to the varied adsorption strength of key reaction intermediates during CO2RR.
Reaction temperature is an important parameter to tune the selectivity and activity of electrochemical CO2 reduction reaction (CO2RR) due to different thermodynamics of CO2RR and competitive hydrogen evolution reaction (HER). In this work, temperature-dependent CO2RR over Fe-N-C and Ni-N-C single-atom catalysts are investigated from 303 to 343 K. Increasing the reaction temperature improves and decreases CO Faradaic efficiency over Fe-N-C and Ni-N-C catalysts at high overpotentials, respectively. CO current density over Fe-N-C catalyst increases with temperature, then gets into a plateau at 323 K, finally reaches the maximum value of 185.8 mA cm(-2) at 343 K. While CO current density over Ni-N-C catalyst achieves the maximum value of 252.5 mA cm(-2) at 323 K, and then drops significantly to 202.9 mA cm(-2) at 343 K. Temperature programmed desorption results and density functional theory calculations reveal that the difference of temperature-dependent variation on CO Faradaic efficiency and current density between Fe-N-C and Ni-N-C catalysts results from the varied adsorption strength of key reaction intermediates during CO2RR.
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