We found that molybdenum carbide (MoC) can be applied as a novel and efficient heterogeneous catalyst for hydrogen transfer of anilines and alcohols to synthesize -alkylamines. The results of experiments and DFT calculations demonstrate that MoC surface can reduce the energy barrier of the key step of alcohol dehydrogenation and generate a hydrogen spillover effect, thereby exhibiting outstanding catalytic performance.
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http://dx.doi.org/10.1039/d4cc04327h | DOI Listing |
Nat Commun
January 2025
Graduate School of Pharmaceutical Sciences, The University of Tokyo, 7-3-1 Hongo, Bunkyo-ku, Tokyo, 113-0033, Japan.
The advancement of an effective hydrogen liberation technology from liquid organic hydrogen carriers, particularly cycloalkanes such as cyclohexane and methylcyclohexane, holds significance in realizing a hydrogen-centric society. However, the attainment of homogeneous catalytic acceptorless dehydrogenation characterized by elevated selectivity for thorough aromatization under mild conditions remains unrealized. In this study, a catalyst system, facilitated by a double hydrogen atom transfer processes, has been devised for the catalytic acceptorless dehydrogenation of inert cycloalkanes at ambient temperature under visible light irradiation.
View Article and Find Full Text PDFJ Org Chem
January 2025
College of Material, Chemistry and Chemical Engineering, Key Laboratory of Organosilicon Chemistry and Material Technology, Ministry of Education, Hangzhou Normal University, Hangzhou 311121, China.
In this study, a novel approach that combines photoinduced electron transfer (ET) with hydrogen atom transfer (HAT) has been introduced for the selective β-C(sp)-H pyridination of carbonyl compounds. This method is notable for its absence of transition metals and its ability to function under benign reaction conditions, resulting in a range of pyridinated carbonyl derivatives with consistently moderate to good yields. The significance of this technique is further underscored by its potential for the late-stage functionalization of pharmaceutically significant molecules.
View Article and Find Full Text PDFJ Org Chem
January 2025
Department of Chemistry, Fudan University, 2005 Songhu Road, Shanghai 200438, P. R. China.
Amino compounds are important molecules, commonly found in nature and widely applied in industrial production. Recently, photocatalysis has been discovered as an efficient method to synthesize amino compounds by promoting imine hydrogenation. In this work, a strategy of imine hydrogenation catalyzed by 2e consecutive photoinduced electron transfer (ConPET) process of thioxanthone-TfOH complex (9-HTXTF) was thoroughly investigated with its reaction conditions optimized, substrate scope examined, and reaction mechanism elucidated, which provides an efficient method for synthesizing amino compounds.
View Article and Find Full Text PDFNanoscale
January 2025
Department of Chemistry, Central University of Kerala, India.
The quest for highly efficient electrocatalysts for direct urea fuel cells (DUFCs) is vital in addressing the energy deficits and environmental crisis. Ni-based LDHs are widely known for their substantial capability in urea oxidation reactions (UOR). This study involved the synthesis of NiCr-LDH/VC MXene nanocomposites (NCVs) and the evaluation of their electrochemical efficiency towards UOR.
View Article and Find Full Text PDFChem Sci
December 2024
Key Laboratory of Precision and Intelligent Chemistry, University of Science and Technology of China Hefei Anhui 230026 China
The packing of organic molecular crystals is often dominated by weak non-covalent interactions, making their rearrangement under external stimuli challenging to understand. We investigate a pressure-induced single-crystal-to-single-crystal (SCSC) transformation between two polymorphs of 2,4,5-triiodo-1-imidazole using machine learning potentials. This process involves the rearrangement of halogen and hydrogen bonds combined with proton transfer within a complex solid-state system.
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