It is a dream of researchers to be able to tailor the catalytic performances by adjusting heterogeneous catalysts at the atomic level. Atomically precise metal clusters provide us with the possibility to achieve this challenge. Here, we design a push-and-pull synthesis strategy coupled with TiO coating to prepare the heterogeneous catalysts denoted as TiO/AuM@SBA via cultivating atomically precise AuM(PPh) (M=Pd, Pt or Au; n=2 for Pd/Pt and 3 for Au) clusters in mesoporous molecular sieve. The catalysts are made up of the three functional units, which include AuM(PPh) clusters that can act as the active sites, the pore environment of the SBA-15 that can announce a catalysis show for the clusters with precise number of atoms maintained during the chemical reactions, and the TiO coating that can further inhibit the migration of the clusters under reaction conditions. The selective hydrogenation of acetylene performed in the fixed-bed reactor taken, for example, we learn how the atom-by-atom tailoring of a heterogeneous catalyst can switch on elusive heterogeneous mechanisms with cluster catalysis. This work sheds light on the fundamental insight into catalysis origin of heterogeneous catalysts and achieves a distinguished level of detail for cluster catalysis.
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http://dx.doi.org/10.1002/anie.202420274 | DOI Listing |
Sci Rep
January 2025
Jadara University Research Center, Jadara University, PO Box 733, Irbid, Jordan.
In this study, the AlFeO@n-Pr@Et-SOH heterogeneous catalyst was successfully synthesized and utilized to produce biodiesel from oleic acid through an esterification process and to oxidize sulfides. To examine the physicochemical characteristics of the AlFeO@n-Pr@Et-SOH nanomaterial, a variety of advanced techniques were employed, including Fourier Transform infrared spectroscopy (FT-IR), Field emission scanning electron microscopy (FE-SEM), Energy dispersive X-ray spectroscopy (EDX), Vibrating sample magnetometer (VSM), Elemental Mapping, Transmission electron microscopy (TEM), Inductively coupled plasma (ICP), and X-ray diffraction (XRD). The AlFeO@n-Pr@Et-SOH materials demonstrated excellent performance in both the esterification of oleic acid and the oxidation of sulfides.
View Article and Find Full Text PDFJ Colloid Interface Sci
December 2024
Guangdong Key Laboratory of Environmental Catalysis and Health Risk Control, School of Environmental Science and Engineering, Institute of Environmental Health and Pollution Control, Guangdong University of Technology, Guangzhou 510006, China.
Developing advanced heterogeneous catalysts through structural modifications effectively enhances the catalytic activity of non-homogeneous catalysts for removing emerging micropollutants (EMPs). In this study, MoTiCT@Co with Mo vacancies was synthesized using the Lewis molten salt method, which efficiently activates peroxymonosulfate (PMS) and continuously degrades EMPs in water. The abundant Mo vacancy structure in the material acts as an anchoring site for Co nanoparticles and a co-catalytic site for Fenton-like reactions, enabling PMS adsorption and activation.
View Article and Find Full Text PDFJ Phys Chem Lett
January 2025
International Tomography Center, SB RAS, 3A Institutskaya St., Novosibirsk 630090, Russia.
Nuclear magnetic resonance is extremely attractive for operando studies of chemical reactors. However, the heterogeneous catalyst particles placed inside an NMR probe greatly affect the uniformity of the magnetic field. This problem is especially acute when studying heterogeneous hydrogenation processes using parahydrogen.
View Article and Find Full Text PDFACS Catal
January 2025
Institute of Chemical and Bioengineering, Department of Chemistry and Applied Biosciences, ETH Zurich, Vladimir-Prelog-Weg, 1, 8093 Zurich, Switzerland.
Buchwald-Hartwig (BH) aminations are crucial for synthesizing arylamine motifs in numerous bioactive molecules and fine chemicals. While homogeneous palladium complexes can be effective catalysts, their high costs and environmental impact motivate the search for alternative approaches. Heterogeneous palladium single-atom catalysts (SAC) offer promising recoverable alternatives in C-C cross-couplings.
View Article and Find Full Text PDFCatal Sci Technol
December 2024
Department of Chemistry, Biochemistry and Pharmaceutical Sciences, University of Bern Freiestrasse 3 3012 Bern Switzerland
Even though α-arylation of ketones is attractive for direct C-H functionalization of organic substrates, the method largely relies on phosphine-ligated palladium complexes. Only recently, efforts have focused on developing nitrogen-based ligands as a more sustainable alternative to phosphines, with pyridine-functionalized pyridinium amidate (pyr-PYA) ,'-bidentate ligands displaying good selectivity and activity. Here, we report on a second generation set of catalyst precursors that feature a 5-membered N-heterocycle instead of a pyridine as chelating unit of the PYA ligand to provide less steric congestion for the rate-limiting transmetalation of the enolate.
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