期刊
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
卷 19, 期 37, 页码 25527-25536出版社
ROYAL SOC CHEMISTRY
DOI: 10.1039/c7cp03914j
关键词
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资金
- Federal Ministry of Education and Research of Germany (BMBF) through the project Strom aus Luft und Li'' [03X4624A]
- MoHE (Egypt)
- DAAD
Understanding the mechanism underlying the oxygen evolution reaction (OER) on oxides is crucial for the development of many energy storage systems. Here, the mechanism of OER on a Co3O4 spinel catalyst is investigated in alkaline media using O-18-labeling combined with differential electrochemical mass spectrometry (DEMS). This work unravels the role of surface oxygen of the oxide in the OER. It is shown that in (H2O)-O-18-containing electrolyte the amount of (18OO)-O-16 evolved increases from cycle to cycle together with a concomitant decrease of the amount of O-16(2) with each cycle before reaching a steady-state value. (OO)-O-18-O-16 is also evolved from a (H2O)-O-16 solution on a Co3O4 electrode pre-treated in (H2O)-O-18-containing solution, indicating the formation of the O-18-labeled oxide in the previous step. Therefore, the oxide layer takes part in OER via an oxygen exchange mechanism. The total number of oxygen atoms of the oxide participating in OER is 0.1 to 0.2% of the total oxide loading, corresponding to about 10-30% of the surface atoms; these represent the catalytically active sites. Moreover, the real surface area of the catalyst is estimated using different methods (namely the ball model, double layer capacitance method, redox peak method, isotope exchange), and compared to the BET data. The surface areas calculated from the BET data, ball model and redox peak method are similar for small particles, which indicates their smooth surface; however they are smaller than that estimated from double-layer capacitance. For larger particles, the much larger surface area estimated from the redox peak in comparison to that expected from the ball model seems to be due to their roughness. Thus, this work highlights the importance of probing the mechanism when investigating the OER activity of a catalyst.
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