Journal
CHEMELECTROCHEM
Volume 5, Issue 5, Pages 805-810Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/celc.201701361
Keywords
oxygen reduction reaction; copper; electrocatalysis; heterogeneous catalysis; nanostructures
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Funding
- NIMS Microstructural Characterization Platform as part of the Nanotechnology Platform program of the Ministry of Education, Culture, Sports, Science and Technology (MEXT), Japan
- PRESTO Program of the Japan Science and Technology Agency (JST) [JPMJPR1415]
- JSPS KAKENHI Program [16 J09552, 17H04798]
- Grants-in-Aid for Scientific Research [16J09552] Funding Source: KAKEN
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This work confirms a trade-off relationship between the high redox potential of Cu and the oxygen-binding ability of Cu-based oxygen reduction reaction (ORR) electrocatalysts. As the ORR is mediated by Cu(I) species, a positive shift of the Cu(II/I) potential is required to increase the ORR onset potential. However, the ready simultaneous autoreduction of Cu(II) to Cu(I) in Cu complexes, owing to high redox potentials, results in the formation of a closed tetrahedral configuration that is inactive for O-2 adsorption and, therefore, for the ORR. To mitigate this problem, we synthesized a Cu-modified S-linked covalent triazine framework (Cu-S-CTF) as an electrocatalyst for the ORR in neutral solutions. The Cu(I) ions in this material have a distorted three-coordinated structure with accessible coordination sites for O-2, because the inflexibility of the CTF suppresses the formation of the tetrahedral configuration. The ORR onset potential of Cu-S-CTF was 880mV versus a reversible hydrogen electrode at pH7. This is the first example of an ORR electrocatalyst containing Cu sites with both high redox potential and oxygen-binding ability.
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