期刊
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
卷 60, 期 33, 页码 18129-18137出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202104148
关键词
carboxylate ligands; catalytic mechanisms; electrocatalysis; layered double hydroxides
资金
- National Basic Research Program of China [2016YFA0202603]
- NSFC [21821003, 91645104]
- Natural Science Foundation of Guangdong Province [S2013020012833, 2016A010104004]
- Guangdong Basic and Applied Basic Research Foundation [2019A1515111033]
- China Postdoctoral Science Foundation [2020M672934]
- Fundamental Research Funds for the Central Universities, Sun Yat-sen University [20lgpy88]
The study revealed the extraordinary role and mechanism of carboxylate ligands on bimetallic/tri-metallic layered double hydroxides/MOFs catalytic activity for the oxygen evolution reaction, enhancing the electrocatalytic performance of OER.
Metal-organic frameworks (MOFs) with carboxylate ligands as co-catalysts are very efficient for the oxygen evolution reaction (OER). However, the role of local adsorbed carboxylate ligands around the in-situ-transformed metal (oxy)hydroxides during OER is often overlooked. We reveal the extraordinary role and mechanism of surface-adsorbed carboxylate ligands on bi/trimetallic layered double hydroxides (LDHs)/MOFs for OER electrocatalytic activity enhancement. The results of X-ray photoelectron spectroscopy (XPS), synchrotron X-ray absorption spectroscopy, and density functional theory (DFT) calculations show that the carboxylic groups around metal (oxy)hydroxides can efficiently induce interfacial electron redistribution, facilitate an abundant high-valence state of nickel species with a partially distorted octahedral structure, and optimize the d-band center together with the beneficial Gibbs free energy of the intermediate. Furthermore, the results of in situ Raman and FTIR spectra reveal that the surface-adsorbed carboxylate ligands as Lewis base can promote sluggish OER kinetics by accelerating proton transfer and facilitating adsorption, activation, and dissociation of hydroxyl ions (OH-).
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