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Synthesis and Performance Characterizations of Transition Metal Single Atom Catalyst for Electrochemical CO2 Reduction
Published on: April 10, 2018
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Carbon Dioxide Promoted H(+) Reduction Using a Bis(imino)pyridine Manganese Electrocatalyst
Tufan K Mukhopadhyay, Nicholas L MacLean, Lu Gan
1‡Department of Chemistry, Indiana University, Bloomington, Indiana 47405, United States.
Inorganic Chemistry
|April 23, 2015
Summary
This study synthesized two manganese complexes, one of which catalyzes CO2 reduction to H2 with high efficiency using methanol. Careful consideration is needed when evaluating manganese complexes for electrocatalytic CO2 reduction.
Area of Science:
- Organometallic Chemistry
- Electrochemistry
- Catalysis
Background:
- Manganese complexes are explored for catalytic applications.
- Pyridine diimine (PDI) ligands offer versatile coordination environments.
- Understanding ligand and metal redox states is crucial for catalytic activity.
Purpose of the Study:
- Synthesize and characterize novel manganese complexes with phosphine-substituted PDI ligands.
- Investigate the electrocatalytic activity of these complexes for CO2 reduction.
- Determine the role of CO2 and proton sources in the catalytic process.
Main Methods:
- Synthesis of manganese complexes via heating reactions.
- Structural characterization using single crystal X-ray diffraction.
- Electrochemical studies including cyclic voltammetry and bulk electrolysis.
- Density functional theory (DFT) calculations for electronic structure analysis.
Main Results:
- Two manganese complexes, [((Ph2PPr)PDI)Mn(CO)][Br] (1) and ((Ph2PPr)PDI)MnBr (2), were synthesized.
- Complex 1 demonstrated electrocatalytic reduction of CO2 to H2 with high Faradaic efficiency (96.7%) in the presence of methanol.
- CO2 was found to promote H2 production by lowering the apparent pH.
- Complex 2 showed limited activity and decomposed rapidly in acidic conditions.
Conclusions:
- The diamagnetic Mn(I) complex 1 is an effective electrocatalyst for CO2 reduction to H2.
- Proton source concentration and CO2 significantly influence the catalytic efficiency.
- The paramagnetic Mn(II) complex 2 is less stable and less effective as a catalyst.
- Further research is needed to optimize manganese complexes for electrocatalytic CO2 reduction, considering stability and reaction conditions.
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