Bisulfate as a redox-active ligand in vanadium-based electrocatalysis for CH4 functionalization.
Danlei Xiang1, Sheng-Chih Lin2, Jiao Deng1
1Department of Chemistry and Biochemistry, University of California Los Angeles, Los Angeles, California 90095, USA. chongliu@chem.ucla.edu.
Chemical Communications (Cambridge, England)
|January 31, 2022
Summary
Sulfuric acid
Area of Science:
- Catalysis
- Inorganic Chemistry
- Electrochemistry
Background:
- Computational studies suggested sulfuric acid's role in methane activation.
- Experimental validation of sulfuric acid's role in methane activation with molecular catalysts is limited.
Purpose of the Study:
- To provide experimental evidence for the role of sulfuric acid in vanadium-based electrocatalytic methane activation.
- To investigate the redox activity of metal-bound bisulfate ligands in this process.
Main Methods:
- Electrocatalytic methane activation using vanadium-oxo dimer pre-catalysts.
- Ligand modification by replacing bisulfate with dihydrogen phosphate.
Main Results:
- Experimental evidence confirms the redox activity of metal-bound bisulfate ligands in vanadium-catalyzed methane activation.
- Replacing bisulfate with a redox-inert dihydrogen phosphate ligand completely inhibited methane activation.
Conclusions:
- The bisulfate ligand, introduced by sulfuric acid, is crucial for the catalytic activity of vanadium-oxo dimers in methane activation.
- This finding suggests potential for developing environmentally benign catalytic systems with reduced reliance on concentrated sulfuric acid.
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