Journal
ADVANCED FUNCTIONAL MATERIALS
Volume 31, Issue 48, Pages -Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/adfm.202106835
Keywords
amorphous shell; deprotonation; electrocatalysis; Prussian blue analogues; transformation
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Funding
- China Scholarship Council
- EPSRC Centre for Doctoral Training in the Advanced Characterization of Materials [EP/L015277/1]
- Imperial College London
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Developing low-cost oxygen evolution reaction (OER) catalysts with high efficiency and understanding the underlying reaction mechanism are critical for electrochemical conversion technologies. A Prussian blue analogue containing Ni and Co was reported as a promising OER electrocatalyst in alkaline media, with detailed characterizations revealing a transformation process from PBA to Ni(OH)(2) and an increase in Ni valence leading to improved adsorption strength of oxygen-containing species. The proposed OER mechanism of the transformed product showed high performance in a water-splitting electrolysis cell with no obvious performance attenuation after 40 hours of catalysis.
Developing low-cost oxygen evolution reaction (OER) catalysts with high efficiency and understanding the underlying reaction mechanism are critical for electrochemical conversion technologies. Here, an anodized Prussian blue analogue (PBA) containing Ni and Co is reported as a promising OER electrocatalyst in alkaline media. Detailed post-mortem characterizations indicate the transformation from PBA to Ni(OH)(2) during the anodic process, with the amorphous shell of the PBA facilitating the transformation by promoting greater structural flexibility. Further study with operando Raman and X-ray photoelectron spectroscopy reveal the increase of anodic potential improves the degree of deprotonation of the transformed core-shell PBA, leading to an increase of Ni valence. Density functional theory calculations suggest that the increase of Ni valence results in a continuous increase in the adsorption strength of oxygen-containing species, exhibiting a volcano relationship against the OER activity. Based on the experiments and calculated results, an OER mechanism for the transformed product is proposed. The fully activated catalyst also works as the cathode and the anode for a water-splitting electrolysis cell with a high output current density of 13.7 mA cm(-2) when a cell voltage of 1.6 V applied. No obvious performance attenuation is observed after 40 h of catalysis.
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