Cobalt–Graphene Catalyst for Selective Hydrodeoxygenation of Guaiacol to Cyclohexanol

Abstract

Herein, cobalt-reduced graphene oxide (rGO) catalyst was synthesized with a practical impregnation–calcination approach for the selective hydrodeoxygenation (HDO) of guaiacol to cyclohexanol. The synthesized Co/rGO was characterized by transmission electron microscopy (TEM), high-angle annular dark-field scanning TEM (HAADF-STEM), X-ray photoelectron spectroscopy (XPS), Raman spectroscopy, X-ray diffraction (XRD), and H2 temperature-programmed reduction (H2-TPR) analysis. According to the comprehensive characterization results, the catalyst contains single Co atoms in the graphene matrix and Co oxide nanoparticles (CoOx) on the graphene surface. The isolated Co atoms embedded in the rGO matrix form stable metal carbides (CoCx), which constitute catalytically active sites for hydrogenation. The rGO material with proper amounts of N heteroatoms and lattice defects becomes a suitable graphene material for fabricating the catalyst. The Co/rGO catalyst without prereduction treatment leads to the complete conversion of guaiacol with 93.2% selectivity to cyclohexanol under mild conditions. The remarkable HDO capability of the Co/rGO catalyst is attributed to the unique metal–acid synergy between the CoCx sites and the acid sites of the CoOx nanoparticles. The CoCx sites provide H while the acid sites of CoOx nanoparticles bind the C-O group of reactants to the surface, allowing easier C-O scission. The reaction pathways were characterized based on the observed reaction–product distributions. The effects of the process parameters on catalyst preparation and the HDO reaction, as well as the reusability of the catalyst, were systematically investigated.

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“…Different reaction pathways existed during hydrotreating process of GAL, such as hydrogenation, demethylation, DMO, and direct dehydration. [ 158 ] Based on previous research, two competing reaction pathways existed in converting GAL into cyclohexanol (Figure 10C): (i) GAL underwent aromatic ring hydrogenation to produce 2‐methoxycyclohexanol, followed by DMO to produce cyclohexanol (pathway III); and (ii) GAL was first converted to phenol by DMO, followed by phenol hydrogenation to produce cyclohexanol (pathway I). At the same time, there was a side reaction (pathway II).…”