In 1994 and again in 2008 Bocarsly announced the discovery of a new stunningly efficient catalyst for the electrochemical reduction of carbon dioxide to formic acid, formaldehyde, and ultimately methanol. In 2010 Bocarsly presented experimental and theoretical mechanistic studies identifying the rate-limiting step as formation of a pyridyl N-C bond bond with CO2 to give a carbamic acid intermediate. We will discuss a general strategy for improving the activity of the catalyst system by rational design of a catalyst for which the activation barrier of this step should be reduced. The synthesis of a series of catalysts, which should have a systematic variation of catalytic activity, will be presented along with preliminary results for assessment of their activity relative to Bocarsly 's original catalyst.
All Science Journal Classification (ASJC) codes
- Chemical Engineering(all)