Inverse ceria-nickel catalyst for enhanced C–O bond hydrogenolysis of biomass and polyether

Abstract

Regulating interfacial electronic structure of oxide-metal composite catalyst for the selective transformation of biomass or plastic waste into high-value chemicals through specific C–O bond scission is still challenging due to the presence of multiple reducible bonds and low catalytic activity. Herein, we find that the inverse catalyst of 4CeO_x/Ni can efficiently transform various lignocellulose derivatives and polyether into the corresponding value-added hydroxyl-containing chemicals with activity enhancement (up to 36.5-fold increase in rate) compared to the conventional metal/oxide supported catalyst. In situ experiments and theoretical calculations reveal the electron-rich interfacial Ce and Ni species are responsible for the selective adsorption of C–O bond and efficient generation of H^δ− species, respectively, which synergistic facilitate cleavage of C–O bond and subsequent hydrogenation. This work advances the fundamental understanding of interfacial electronic interaction over inverse catalyst and provides a promising catalyst design strategy for efficient transformation of C–O bond.