Construction of Highly Active and Selective Molecular Imprinting Catalyst for Hydrogenation.
Dongcheng HeTeng LiXingchao DaiShujuan LiuXinjiang CuiFeng ShiPublished in: Journal of the American Chemical Society (2023)
Surface molecular imprinting (MI) is one of the most efficient techniques to improve selectivity in a catalytic reaction. Heretofore, a prerequisite to fabricating selective catalysts by MI strategies is to sacrifice the number of surface-active sites, leading to a remarkable decrease of activity. Thus, it is highly desirable to design molecular imprinting catalysts (MICs) in which both the catalytic activity and selectivity are significantly enhanced. Herein, a series of MICs are prepared by sequentially adsorbing imprinting molecules (nitro compounds, N ) and imprinting ligand (1,10-phenanthroline, L ) over the copper surface of Cu/Al 2 O 3 . The resulting Cu/Al 2 O 3 -N-L MICs not only offer promoted catalytic selectivity but also enhance catalytic activity for nitro compounds hydrogenation by an creating imprinting cavity derived from the presorption of N and forming new active Cu-N sites at the interface of the copper sites and L . Characterizations by means of various experimental investigations and DFT calculations disclose that the molecular imprinting effect (promoted activity and selectivity) originates from the formation of new active Cu-N sites and precise imprinting cavities, endowing promoted catalytic selectivity and activity on the hydrogenation of nitro compounds.