| Autor: |
Ze, Huajie, Yang, Zhi-Lan, Li, Mu-Lin, Zhang, Xia-Guang, A, Yao-Lin, Zheng, Qing-Na, Wang, Yao-Hui, Tian, Jing-Hua, Zhang, Yue-Jiao, Li, Jian-Feng |
| Zdroj: |
Journal of the American Chemical Society; May 2024, Vol. 146 Issue: 18 p12538-12546, 9p |
| Abstrakt: |
There is growing acknowledgment that the properties of the electrochemical interfaces play an increasingly pivotal role in improving the performance of the hydrogen evolution reaction (HER). Here, we present, for the first time, direct dynamic spectral evidence illustrating the impact of the interaction between interfacial water molecules and adsorbed hydroxyl species (OHad) on the HER properties of Ni(OH)2using Au/core-Ni(OH)2/shell nanoparticle-enhanced Raman spectroscopy. Notably, our findings highlight that the interaction between OHadand interfacial water molecules promotes the formation of weakly hydrogen-bonded water, fostering an environment conducive to improving the HER performance. Furthermore, the participation of OHadin the reaction is substantiated by the observed deprotonation step of Au@2 nm Ni(OH)2during the HER process. This phenomenon is corroborated by the phase transition of Ni(OH)2to NiO, as verified through Raman and X-ray photoelectron spectroscopy. The significant redshift in the OH-stretching frequency of water molecules during the phase transition confirms that surface OHaddisrupts the hydrogen-bond network of interfacial water molecules. Through manipulation of the shell thickness of Au@Ni(OH)2, we additionally validate the interaction between OHadand interfacial water molecules. In summary, our insights emphasize the potential of electrochemical interfacial engineering as a potent approach to enhance electrocatalytic performance. |
| Databáze: |
Supplemental Index |
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