The production of biofuel 2,5-dimethylfuran (DMF) from an important biomass platform of 5-hydroxymethyl furfural (HMF) involves a complicated reaction pathway due to the competition of C=O hydrogenation and C-O hydrogenolysis; however, the dependence of formed intermediates and catalytic sites needs to be further identified. Herein, we constructed a highly efficient and selective Cu/ZnO-Al2O3 catalyst via reduction of a CuZnAl-layer double hydroxide (LDH) precursor, aimed for studying the effect of Cu-0/Cu+ species on forming different intermediates and their synergetic promotional effect on HMF hydrodeoxygenation. As expected, the dependence of formation of different intermediates on the Cu+/Cu-0 ratio was observed; notably, Cu/ZnOAl2O3 with higher Cu+/Cu-0 ratio finally gave 90.1% DMF selectivity at 100% HMF conversion, more selective than CuNi/(AlO3)-O-2 (59.6%) and Cu/MgO-Al2O3 (75.8%) references. By a combined study of in situ IR experiments, the observed correlation between the reaction intermediates and the Cu-0/Cu+ site suggests that Cu-0 tends to adsorb the C=O bond as well as hydrogen molecule, while the Cu+ site is preferable to adsorb and activate the C-O bond. With the synergy of dual active sites, the Cu/ZnO-(AlO3)-O-2 catalyst showed both high activity and selectivity to DMF. This work provides deep insight into the nature of active Cu species in multiple functional group biomass platform transformation.
Insight into the Effect of Dual Active Cu-0/Cu+ Sites in a Cu/ZnO-Al2O3 Catalyst on 5-Hydroxylmethylfurfural Hydrodeoxygenation
Fornasiero, P;
2020-01-01
Abstract
The production of biofuel 2,5-dimethylfuran (DMF) from an important biomass platform of 5-hydroxymethyl furfural (HMF) involves a complicated reaction pathway due to the competition of C=O hydrogenation and C-O hydrogenolysis; however, the dependence of formed intermediates and catalytic sites needs to be further identified. Herein, we constructed a highly efficient and selective Cu/ZnO-Al2O3 catalyst via reduction of a CuZnAl-layer double hydroxide (LDH) precursor, aimed for studying the effect of Cu-0/Cu+ species on forming different intermediates and their synergetic promotional effect on HMF hydrodeoxygenation. As expected, the dependence of formation of different intermediates on the Cu+/Cu-0 ratio was observed; notably, Cu/ZnOAl2O3 with higher Cu+/Cu-0 ratio finally gave 90.1% DMF selectivity at 100% HMF conversion, more selective than CuNi/(AlO3)-O-2 (59.6%) and Cu/MgO-Al2O3 (75.8%) references. By a combined study of in situ IR experiments, the observed correlation between the reaction intermediates and the Cu-0/Cu+ site suggests that Cu-0 tends to adsorb the C=O bond as well as hydrogen molecule, while the Cu+ site is preferable to adsorb and activate the C-O bond. With the synergy of dual active sites, the Cu/ZnO-(AlO3)-O-2 catalyst showed both high activity and selectivity to DMF. This work provides deep insight into the nature of active Cu species in multiple functional group biomass platform transformation.File | Dimensione | Formato | |
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