Catalytic Strategies for the Reductive Functionalization of CO$_2$
Abstract
While greenhouse gases emissions are reaching alarming levels, fossil fuels still represent 80% of the world energy portfolio and 95% of our chemical commodities rely on non-renewable resources, namely hydrocarb'bns. In this context, utilizing CO$_2$ as a C$_l$ building block to pro duce platform chemicals as an alternative to petrochemistry has a double advantage of reusing CO$_2$ while sparing fossil resources and avoiding CO$_2$ emissions from their use. We have developed a strategy relying on the simultaneous use of a functionalizing reagent and a reductant that can be $independently$ adjusted to perform the reductive functionalization of CO$_2$. The so-called $diagonal\ approach$ will be discussed and exemplified with novel catalytic processes to convert CO$_2$ to formamides, N-heterocycIes, methylamines and methanol, using hydroboranes, hydrosilanes or formic acid as reductants. These new catalytic reactions rely on the use of simple organocatalysts or Zn, Fe and Ru organometallic complexes. The mechanisms at play in these transformations will be presented, based on DFT caIculations and isolation ofreactive catalytic intermediates.
Domains
Material chemistry
Origin : Files produced by the author(s)
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