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Metal-organic frameworks (MOFs) with carboxylate ligands as co-catalysts are very efficient for 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. Here we reveal the extraordinary role and mechanism of surface adsorbed carboxylate ligands on bi/trimetallic layered double hydroxides (LDHs)/MOFs for OER catalytic activity enhancement. The results of X-ray photoelectron spectroscopy (XPS), synchrotron X-ray absorption spectroscopy and theoretical calculations show that the carboxylic groups around metal (oxy)hydroxides can efficiently induce the interfacial electron redistribution, facilitate abundant high-valence state of nickel species with partial distorted octahedral structure, and optimize the d-band center together with the beneficial Gibbs free energy of intermediate. Furthermore, the results of in-situ Raman and FI-IR spectra firstly reveal that the surface adsorbed carboxylate ligands as Lewis base can promote the sluggish OER kinetics by accelerating proton transfer and facilitating adsorption/ activation/dissociation of hydroxyl ions (OH−). Our findings will offer unique insights into the reason for disclosing the origin of excellent electrocatalytic activity for MOF/NiFe-LDHs catalysts.
Keywords
Metal-organic frameworks, Carboxylate ligands, Oxygen evolution reaction, Electrocatalysis, NiFe LDHs
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There is NO Competing Interest.
This is a list of supplementary files associated with this preprint. Click to download.
- NiFeMIL53SI.docx
Supporting information
- Scheme1.pdf
Scheme 1. Promoted OER activity of metal oxyhydroxides via either inherent or extra addition carboxylates.
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This is a preprint, a preliminary version of a manuscript that has not completed peer review at a journal. Research Square does not conduct peer review prior to posting preprints. The posting of a preprint on this server should not be interpreted as an endorsement of its validity or suitability for dissemination as established information or for guiding clinical practice.
Article
Badges
Prescreen
This manuscript passed our Prescreen assessment
Complete author information
Appropriate declaration statements
Potential risks to human health
Prescreen
History
CURRENT STATUS: Posted
Version 1
Posted 08 Feb, 2021
No community comments so far
Metrics
Comments: 0
PDF Downloads: ...
HTML Views: ...
License:
This work is licensed under a CC BY 4.0 License. Read Full License
Metal-organic frameworks (MOFs) with carboxylate ligands as co-catalysts are very efficient for 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. Here we reveal the extraordinary role and mechanism of surface adsorbed carboxylate ligands on bi/trimetallic layered double hydroxides (LDHs)/MOFs for OER catalytic activity enhancement. The results of X-ray photoelectron spectroscopy (XPS), synchrotron X-ray absorption spectroscopy and theoretical calculations show that the carboxylic groups around metal (oxy)hydroxides can efficiently induce the interfacial electron redistribution, facilitate abundant high-valence state of nickel species with partial distorted octahedral structure, and optimize the d-band center together with the beneficial Gibbs free energy of intermediate. Furthermore, the results of in-situ Raman and FI-IR spectra firstly reveal that the surface adsorbed carboxylate ligands as Lewis base can promote the sluggish OER kinetics by accelerating proton transfer and facilitating adsorption/ activation/dissociation of hydroxyl ions (OH−). Our findings will offer unique insights into the reason for disclosing the origin of excellent electrocatalytic activity for MOF/NiFe-LDHs catalysts.
Figure 1
Figure 2
Figure 3
Figure 4
Figure 5
Figure 6
There is NO Competing Interest.
This is a list of supplementary files associated with this preprint. Click to download.
- NiFeMIL53SI.docx
Supporting information
- Scheme1.pdf
Scheme 1. Promoted OER activity of metal oxyhydroxides via either inherent or extra addition carboxylates.
- TableofContentsGraphic.jpg
Table of Contents graphic
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