CO₂Fixation into Organic Molecules via Carbon–Heteroatom Bond Formation

Electrochemical Reductive N-Methylation with CO2 Enabled by a Molecular Catalyst

“…An active goal in synthetic chemistry is the development of methods that incorporate CO 2 as a one-carbon (C1) chemical building block. , A fundamental challenge for this technology is the high thermodynamic stability and kinetic inertness of CO 2 toward desirable chemical transformations. Electrochemical reduction is an attractive approach to sustainably electrosynthesize simple carbon species, such as carbon monoxide (CO), formate, methane, ethylene, methanol (CH 3 OH), and ethanol, from CO 2 . − Although these products are useful, it is desirable to broaden the product scope because many valuable chemicals contain heteroatoms. , Utilizing electrochemical reduction to activate CO 2 for in situ chemical coupling reactions with heteroatom substrates remains largely unexplored. In particular, the activation of CO 2 for carbon–nitrogen (C–N) bond-forming reactions is of interest, because organonitrogen molecules are ubiquitous in the chemical industry. , Previous reports have demonstrated electrochemical C–N bond formation during CO 2 electrolysis with nitrate (NO 3 – ), nitrite (NO 2 – ), or molecular nitrogen (N 2 ) as the nitrogen source, and the product is urea in each case. − When CO is used as the carbon source, and ammonia (NH 3 ) or amines as the nitrogen source, acetamides are the product over a copper electrocatalyst …”