Abstract
The development of precious-metal-free catalysts to promote the sustainable production of fuels and chemicals from biomass remains an important and challenging target. Here, we report the efficient hydrogenolysis of biomass-derived 5-hydroxymethylfurfural to 2,5-dimethylfuran over a unique core-shell structured catalyst, Co@CoO that affords the highest productivity among all catalysts, including noble-metal-based catalysts, reported to date. Surprisingly, we find that the catalytically active sites reside on the shell of CoO with oxygen vacancies rather than the metallic Co. The combination of various spectroscopic experiments and computational modelling reveals that the CoO shell incorporating oxygen vacancies not only drives the heterolytic cleavage, but also the homolytic cleavage of H2 to yield more active Hδ− species, resulting in the exceptional catalytic activity. Co@CoO also exhibits excellent activity toward the direct hydrodeoxygenation of lignin model compounds. This study unlocks, for the first time, the potential of simple metal-oxide-based catalysts for the hydrodeoxygenation of renewable biomass to chemical feedstocks.
| Original language | English |
|---|---|
| Article number | 3657 |
| Journal | Nature Communications |
| Volume | 13 |
| Issue number | 1 |
| DOIs | |
| State | Published - Dec 2022 |
Funding
This project was supported financially by the National Natural Science Foundation of China (No. 21832002, 21825301, 21872050, 21808063, 22002043), Shanghai Municipal Science and Technology Major Project (Grant No.2018SHZDZX03), the Programme of Introducing Talents of Discipline to Universities (B16017), China and EPSRC (EP/V056409), UK. This research used Beamline VISION at the Spallation Neutron Source, a DOE Office of Science User Facility operated by the Oak Ridge National Laboratory. This project was supported financially by the National Natural Science Foundation of China (No. 21832002, 21825301, 21872050, 21808063, 22002043), Shanghai Municipal Science and Technology Major Project (Grant No.2018SHZDZX03), the Programme of Introducing Talents of Discipline to Universities (B16017), China and EPSRC (EP/V056409), UK. This research used Beamline VISION at the Spallation Neutron Source, a DOE Office of Science User Facility operated by the Oak Ridge National Laboratory.
