Litcius/Paper detail

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

Bing Lü, Shuangxiu Ma, Shipan Liang, Zhe Wang, Yali Liu, Shanjun Mao, Heng Ban, Lihua Wang, Yong Wang

2023ACS Catalysis27 citationsDOI

Abstract

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.

Topics & Concepts

DehydrogenationCatalysisChemistryButanolBase (topology)Combinatorial chemistryEthanolPhotochemistryOrganic chemistryMathematicsMathematical analysisAsymmetric Hydrogenation and CatalysisCatalytic Processes in Materials ScienceCatalysis for Biomass Conversion