Efficient Conversion of Ethanol to 1-Butanol over Adjacent Acid–Base Dual Sites Via Enhanced C–H Activation

We have developed a composite catalyst featuring acid and base interface that enables the efficient conversion of ethanol to butanol. Our catalyst, which possesses adjacent acid- base sites, exhibits over a eightfold increase in dehydrogenation and condensation rates per site compared to physical mixture of acid and base. This demonstrates a remarkable acid-base synergistic effect in these two kinetically relevant steps. Through isotope experiments, we have elucidated the chemical origin of the strong activation of the C-H bond under cooperative catalysis, which is the transformation of the dehydrogenation mechanism from the "ethoxide pathway", involving basic sites, to the "enolate pathway", involving dual-sites. This work provides valuable insights into the design of catalysts for C-H activation.