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A bioinspired molybdenum-copper molecular catalyst for CO₂ electroreduction.

Ahmed Mouchfiq¹, Tanya K Todorova¹, Subal Dey^1,2

¹Laboratoire de Chimie des Processus Biologiques , UMR 8229 CNRS , Collège de France , Sorbonne Universitè , 11 Place Marcelin Berthelot , 75231 Paris Cedex 05 , France .

Chemical Science

|September 3, 2020

Summary

This study introduces a non-noble metal catalyst for electrocatalytic reduction of carbon dioxide (CO2) to formate. The bimetallic complex acts as a pre-catalyst, forming an active Mo-hydride species for efficient CO2 conversion.

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Area of Science:

Inorganic Chemistry
Electrochemistry
Catalysis

Background:

Development of non-noble metal molecular catalysts for CO2 electroreduction is crucial for sustainable chemistry.
Mimicking active sites of enzymes like carbon monoxide dehydrogenase (CODH2) offers a promising strategy for catalyst design.

Purpose of the Study:

To investigate the electrocatalytic reduction of carbon dioxide (CO2) to formate using a bimetallic Mo-Cu complex.
To elucidate the catalytic mechanism and identify the active species involved in the CO2 reduction process.

Main Methods:

Electrochemical reduction of a bimetallic complex, [(bdt)MoVI(O)S2CuICN]2-.
Infrared spectroelectrochemistry (IR-SEC) for in-situ characterization.
Density functional theory (DFT) computations to understand reaction pathways.

Main Results:

The bimetallic complex functions as a pre-catalyst, requiring reduction to generate the active species.
A Mo-hydride intermediate is formed upon reduction and protonation, which directly reacts with CO2.
The catalytic cycle involves oxo-transfer and subsequent hydride transfer steps.

Conclusions:

The study reveals a novel catalytic pathway for CO2 electroreduction mediated by a Mo-Cu complex.
Findings highlight the potential of metal oxo precursors in designing efficient electrocatalysts for CO2 conversion.
The identified Mo-hydride intermediate provides insights for future catalyst development.