Copper nanoparticle-based catalysts have been extensively applied in industry, but the nanoparticles tend to sinter into larger ones in the chemical atmospheres, which is detrimental to catalyst performance. In this work, we used dealuminated Beta zeolite to support copper nanoparticles (Cu/Beta-deAl) and showed that these particles become smaller in methanol vapor at 200°C, decreasing from ~5.6 to ~2.4 nanometers in diameter, which is opposite to the general sintering phenomenon. A reverse ripening process was discovered, whereby migratable copper sites activated by methanol were trapped by silanol nests and the copper species in the nests acted as new nucleation sites for the formation of small nanoparticles. This feature reversed the general sintering channel, resulting in robust catalysts for dimethyl oxalate hydrogenation performed with supported copper nanoparticles for use in industry.
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http://dx.doi.org/10.1126/science.adj1962 | DOI Listing |
Nat Commun
October 2024
Chemical Sciences Division, Oak Ridge National Laboratory, Oak Ridge, TN, USA.
Chem Asian J
October 2024
Department of Chemical and Biomolecular Engineering, School of Energy Science and Engineering, Vidyasirimedhi Institute of Science and Technology, Rayong, 21210, Thailand.
The rational design of isolated metals containing zeolites is crucial for the catalytic conversion of biomass-derived compounds. Herein, we explored the insertion behavior of the isomorphic substitution of Ti(IV) in different zeolite frameworks, including ZSM-35 (FER), ZSM-5, and BEA. The different aluminium topological densities of each zeolite framework lead to the creation of different degrees of vacant sites for hosting the tetrahedrally coordinated Ti(IV) active sites.
View Article and Find Full Text PDFRSC Adv
July 2024
Department of Chemistry, School of Advanced Sciences, Vellore Institute of Technology Vellore 632014 India
Furfural is a biomass-derived platform molecule that can be converted into a variety of useful products. Catalysts having appropriate balance between Lewis and Brønsted acid sites are suitable for valorisation of furfural. Lewis acidic metal ion incorporated zeolites were studied for this purpose.
View Article and Find Full Text PDFChem Sci
May 2024
The Gene & Linda Voiland School of Chemical Engineering and Bioengineering, Washington State University Pullman WA 99164 USA
The selective formation of C-C bonds, coupled with effective removal of oxygen, plays a crucial role in the process of upgrading biomass-derived oxygenates into fuels and chemicals. However, co-feeding reactants with water is sometimes necessary to assist binding sites in catalytic reactions, thereby achieving desirable performance. Here, we report the design of a CeSnBeta catalyst featuring dual Lewis acidic sites for the efficient production of isobutene from acetone C-C coupling followed by deoxygenation.
View Article and Find Full Text PDFJ Colloid Interface Sci
June 2024
School of Chemistry and Chemical Engineering, Dezhou University, Dezhou 253023, PR China.
Dealuminated Beta zeolite has a large amount of silanol defects on its interface, which provides an ideal place for embedding metal species and creating metal active sites in a confined microenvironment. The confined metal sites as well as their surroundings are closely related to the reactant activation and transient state achievement. Hence, unraveling the confined metal sites is of great significance for the catalytic reaction process.
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