Journal
NANO ENERGY
Volume 57, Issue -, Pages 644-652Publisher
ELSEVIER
DOI: 10.1016/j.nanoen.2018.12.094
Keywords
Controllable tuning; Co-Fe-N nanosheets; Oxygen evolution reaction; Volcano - like trend; Co-Fe sites
Categories
Funding
- National Natural Science Foundation of China [21571089, 51571125, 21503102]
- 111 project [B12015]
- Fundamental Research Funds for the Central Universities [lzujbky-2018-k08, lzujbky-2016-k02, lzujbky-2017-115, lzujbky-2017-it42, lzujbky-2018-it40]
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Transition-metal nitrides (TMNs), especially iron-based TMNs, have high electrical conductivity, superior chemical stability and unique oxygen-reaction ability, and have emerged as a new form of noble metal-free electrocatalysts. In this paper, we demonstrate that the ORR-active/OER-inert single function catalyst Fe-N can be made as the OER/ORR-active bifunctional catalyst Co-Fe-N by controlled substitution of Fe with Co. To obtain atomic insights of the Co-enhanced OER catalysis, we develop a new exfoliation method to prepare atomically thin (1.1 nm) nanosheets (NSs) of CoxFe1-xN0.5 (x = 0, 0.05, 0.1, 0.15 and 0.2). Our studies show that both electronic structure and local binding environment of Fe are modified by Co substitution and the Co-Fe-N NSs show a volcano-like OER catalysis with Co0.15Fe0.85N0.5 NSs being the most efficient OER catalyst, showing the lowest overpotential of 266 mV at 10 mA cm(-2), a Tafel slope of similar to 30 mV dec(-1), and excellent stability in the 1.0 M KOH OER condition. Density functional theory (DFT) calculations suggest that the Co-Fe sites in the Co0.15Fe0.85N0.5 structure are optimized to promote OH* to O* conversion, O*-O* coupling and O-2 formation. The Co0.15Fe0.85N0.5 NSs are a class of new noble-metal-free catalyst for OER.
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