Synergetic effect of Cu0 −Cu+ derived from layered double hydroxides toward catalytic transfer hydrogenation reaction

As a safe and environmentally friendly selective hydrogenation method, catalytic transfer hydrogenation (CTH) has aroused great interest in preparation of high-value-added products from biomass derived resources. Herein, a Cu-based catalyst (Cu/CuAl-MMO-400) was prepared by structural topological transformation of layered double hydroxides (LDHs) precursor, which displayed promising catalytic behavior toward CTH reaction of furfural (FAL) with 2-propanol (2-POL) as the hydrogen donor. Notably, the reaction rate is as high as 0.125 mol g −1 h −1 , which is superior to previously reported non-noble metal catalysts. A combination investigation based on XPS, XANES and Bader charge confirms the co-existence of Cu 0 and Cu + sites on the surface of Cu nanoparticles . Both experimental studies ( in situ DRIFTS and isotope labelling MS) and DFT calculations reveal that the Cu 0 − Cu + synergistic effect plays a vital role in determining catalytic behavior: the Cu + species acts as both dehydrogenation and hydrogenation active site; while the Cu 0 site promotes the transfer of H atoms between adsorbed substrates. This work substantiates a Cu 0 −Cu + synergetic catalysis by establishing structure-property correlation and revealing reaction pathway, which could be extended to other CTH reactions in the upgrading processes of biomass.