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Benefits of active site proximity in Cu@UiO-66 catalysts for efficient upgrading of ethanol to n-butanol
- Source :
- Sustainable Energy & Fuels. 5:4628-4636
- Publication Year :
- 2021
- Publisher :
- Royal Society of Chemistry (RSC), 2021.
-
Abstract
- The upgrading of ethanol to n-butanol converts abundant bioethanol to a better gasoline replacement; however, as a representative tandem reaction it requires the presence of multiple types of active sites in one catalyst, which imposes a great challenge on the synthesis of catalysts. Although a variety of heterogeneous catalysts have been explored in this reaction, the development of efficient catalysts remains sluggish due to the limited knowledge of active sites. Herein, we demonstrated that by using Cu@UiO-66 catalysts with distinctive structures, two kinds of sites were identified: internal Cu metal sites and Lewis acid–oxygen vacancy pairs (Zr3–□) of Zr nodes in the pores of UiO-66 are the active sites, whereas Cu metal sites and Zr nodes on the external surface of UiO-66 are less involved in the upgrading of ethanol to n-butanol. And the intimate contact between internal Cu metal sites and Zr3–□ dictates the key step reactions, namely ethanol dehydrogenation, acetaldehyde condensation, and crotonaldehyde hydrogenation. Benefiting from this proximity, a high yield of n-butanol (22.2%) with negligible amounts of gaseous products could be obtained, which ranks Cu@UiO-66 catalysts among the best state-of-the-art Cu-based catalysts thus giving them great potential applications in industry.
- Subjects :
- biology
Renewable Energy, Sustainability and the Environment
Acetaldehyde
Energy Engineering and Power Technology
Active site
Combinatorial chemistry
Catalysis
chemistry.chemical_compound
Fuel Technology
chemistry
Cascade reaction
n-Butanol
Yield (chemistry)
biology.protein
Dehydrogenation
Crotonaldehyde
Subjects
Details
- ISSN :
- 23984902
- Volume :
- 5
- Database :
- OpenAIRE
- Journal :
- Sustainable Energy & Fuels
- Accession number :
- edsair.doi...........1dbe9514caacff90727e088775a98a2f