Microreactors attract a significant interest for chemical synthesis due to the benefits of small scales such as high surface to volume ratio, rapid thermal ramping, and well-understood laminar flows. The suitability of atomic layer deposition for application of both the nanoparticle catalyst and the support material on the surfaces of channels of microfabricated silicon microreactors is demonstrated in this research. Continuous-flow hydrogenation of propene into propane at low temperatures with TiO -supported catalytic Pt nanoparticles was used as a model reaction. Reaction yield and mass transport were monitored by high-sensitivity microcoil NMR spectroscopy as well as time-of-flight remote detection NMR imaging. The microreactors were shown to be very efficient in propene conversion into propane. The yield of 100 % was achieved at 50 °C with a reactor decorated with Pt nanoparticles of average size of roughly 1 nm and surface coverage of 3.2 % in 20 mm long reaction channels with a residence time of 1100 ms. The activity of the Pt catalyst surfaces was on the order of several to tens of mmol s m .
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http://dx.doi.org/10.1002/chem.201703391 | DOI Listing |
J Am Chem Soc
January 2025
Molecular Synthesis Center, Key Laboratory of Marine Drugs of Ministry of Education, Shandong Key Laboratory of Glycoscience and Glycotherapeutics, School of Medicine and Pharmacy, Ocean University of China, Qingdao 266003, China.
2-Deoxy-β-glycosides are essential components of natural products and pharmaceuticals; however, the corresponding 2-deoxy-β-glycosidic bonds are challenging to chemically construct. Herein, we describe an efficient catalytic protocol for synthesizing 2-deoxy-β-glycosides via either IPrAuNTf-catalyzed activation of a unique 1,2--positioned C2--propargyl xanthate (OSPX) leaving group or (PhO)PAuNTf-catalyzed activation of a 1,2--C2--alkynylbenzoate (OABz) substituent of the corresponding thioglycosides. These activation processes trigger 1,2-alkyl/arylthio-migration glycosylation, enabling the synthesis of structurally diverse 2-deoxy-β-glycosides under mild reaction conditions.
View Article and Find Full Text PDFChem Rev
January 2025
Center for Theoretical Interdisciplinary Sciences Wenzhou Institute, University of Chinese Academy of Sciences, Wenzhou, Zhejiang 325001, P. R. China.
Nanozymes have shown significant potential in cancer catalytic therapy by strategically catalyzing tumor-associated substances and metabolites into toxic reactive oxygen species (ROS) , thereby inducing oxidative stress and promoting cancer cell death. However, within the complex tumor microenvironment (TME), the rational design of nanozymes and factors like activity, reaction substrates, and the TME itself significantly influence the efficiency of ROS generation. To address these limitations, recent research has focused on exploring the factors that affect activity and developing nanozyme-based cascade catalytic systems, which can trigger two or more cascade catalytic processes within tumors, thereby producing more therapeutic substances and achieving efficient and stable cancer therapy with minimal side effects.
View Article and Find Full Text PDFEnzymatic asymmetric synthesis of l-phenylglycine by amino acid dehydrogenases has potential for industrial applications; however, this is hindered by their low catalytic efficiency toward high-concentration substrates. We identified and characterized a novel leucine dehydrogenase (LeuDH) with a high catalytic efficiency for benzoylformic acid via directed metagenomic approaches. Further, we obtained a triple-point mutant LeuDH-EER (D332E/G333E/L334R) with improved stability and catalytic efficiency through the rational design of distal loop 13.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
January 2025
Sichuan University, School of Chemical Engineering, No.24 South Section 1, Yihuan Road, 610065, Chengdu, CHINA.
Covalent organic frameworks (COFs) are often employed in oxygen reduction reactions (ORR) for hydrogen peroxide production due to their tunable structures and compositions. However, COF electrocatalysts require precise structural engineering, such as heteroatoms or metal site doping, to modulate the reaction pathway during the ORR process. In this work, we designed a tetraphenyl-p-phenylenediamine based COF electrocatalyst, namely TPDA-BDA, which exhibited excellent two-electron (2e) ORR performance with high H2O2 selectivity of 89.
View Article and Find Full Text PDFNano Lett
January 2025
Institute of Nanochemistry and Nanobiology, School of Environmental and Chemical Engineering, Shanghai University, Shanghai 200444, P.R. China.
Crystals with three-dimensional (3D) stereoscopic structures, characterized by diverse shapes, crystallographic planes, and morphologies, represent a significant advancement in catalysis. Differentiating and quantifying the catalytic activity of specific surface facets and sites at the single-particle level is essential for understanding and predicting catalytic performance. This study employs super-resolution radial fluctuations electrogenerated chemiluminescence microscopy (SRRF-ECLM) to achieve high-resolution mapping of electrocatalytic activity on individual 3D CuO crystals, including cubic, octahedral, and truncated octahedral structures.
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