Higher
alcohol synthesis (HAS) from biomass-derived syngas (CO/H2) is of considerable interest but has a challenge to achieve
a satisfying yield, as it is a competitive reaction between C–C
coupling and CO insertion. Herein, we employed a solvent (dihydric
alcohol) coordination-assisted impregnation strategy to synthesize
a series of catalysts with Cu and Co encapsulated in ordered mesoporous
SiO2 (denoted as CuCo@M-SiO2). This synthesis
strategy could effectively anchor Cu and Co cations at a close distance
owing to the solvent coordination effect. Additionally, the carbon
derived from the thermal decomposition (inert atmosphere) of the solvent
ligand portrayed a critical role in in situ reduction
of Cu and Co species and synchronous confinement. It also helped structural
dispersant (“spacer”) and inhibited the aggregation
of Cu nanoparticles (NPs). The as-prepared CuCo@M-SiO2 catalyst
contained multiple types of synergistic active sites (Cu0, Co0, and Co
n+) that collaborated
with each other to enhance the higher alcohol yield. It is confirmed
that the CO conversion and higher alcohol selectivity were closely
related to solvent-assisted ligands. Among the selected solvent ligands
(ethylene glycol, 1,2-propanediol, and 1,4-butanediol), the CuCo@M-SiO2 catalyst derived from 1,2-propanediol-assisted impregnation
exhibited a remarkably catalytic performance because of the appropriate
confinement effect with smaller CuCo NPs. Notably, the CO conversion
was as high as 82.2% with space–time yield toward 16.1 mmol
gcat
–1 h–1 of ethanol.
A narrow alcohol distribution of C1–C3-mixed alcohols was over 97.2%. These synthetic strategies may provide
new avenues for designing effective and stable catalysts for HAS.