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This paper reports the first example of C-H arylation of benzene under mild conditions, using H as an electron source {turnover numbers (TONs)=0.7-2.0 for 24 h}. The reaction depends on a Rh-based electron storage catalyst, and proceeds at room temperature and in aqueous solution. Furthermore, the H is inactive during the radical transfer step, greatly reducing unwanted side reactions.
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http://dx.doi.org/10.1002/chem.202102735 | DOI Listing |
J Am Chem Soc
September 2025
State Key Laboratory of Chemistry for NBC Hazards Protection, College of Chemistry, Fuzhou University, Fuzhou 350116, P. R. China.
The activation of methane and other gaseous hydrocarbons at low temperature remains a substantial challenge for the chemistry community. Here, we report an anaerobic photosystem based on crystalline borocarbonitride (BCN) supported Fe-O nanoclusters, which can selectively functionalize C-H bonds of methane, ethane, and higher alkanes to value-added organic chemicals at 12 °C. Scanning transmission electron microscopy and X-ray absorption spectroscopy corroborated the ultrafine FeOOH and FeO species in Fe-O clusters, which enhanced the interfacial charge transfer/separation of BCN as well as the chemisorption of methane.
View Article and Find Full Text PDFACS Omega
August 2025
Departamento de Química, Instituto de Ciências Exatas, Universidade Federal de Minas Gerais, Belo Horizonte, Minas Gerais 31270-901, Brazil.
A Pd-mediated C-H activation methodology was developed for the direct arylation of quinoidal skeletons, both by means of homogeneous catalysis and heterogeneous catalysis using metal-decorated carbon nanotubes, enabling the direct functionalization of quinones in moderate to excellent yields. The derivatives obtained were tested against trypomastigote forms of , showing promising biological activity.
View Article and Find Full Text PDFOrg Lett
August 2025
Department of Chemistry, The University of Hong Kong, Pokfulam Road, Hong Kong, China.
Azulene-fused molecular carbons have sparked intense research interest in recent years. Herein, we report a facile three-step synthesis of azuleno[1,2,3-]phenalene (AzPn), a fused system combining azulene and phenalene units, achieving an overall yield of 39.7%.
View Article and Find Full Text PDFLangmuir
August 2025
College of Chemistry and Environmental Science, Inner Mongolia Key Laboratory of Green Catalysis, Inner Mongolia Normal University, Hohhot 010022, China.
Here, we demonstrated that γ-AlO-supported palladium nanoparticles containing dominant metallic-state Pd sites and charged Pd (Pd and Pd) sites are a highly active, selective, and stable heterogeneous catalyst for a variety of Suzuki-Miyaura-type C(sp)-H or C(sp)-H arylation reactions, resulting in a high cumulative turnover number (TON) of 226 after 6 runs. Multi-technique characterization data, including X-ray absorption fine structure (XAFS) analyses, showed that both the strong metal-support interaction (SMSI) with Pd-O coordination and the fitting increase of metal-metal bonds after reaction efficiently limit Pd leaching and Pd aggregates. The support concerted metalation-deprotonation (SCMD) effect of Pd/γ-AlO is more favorable for the proceeding of the Pd/Pd catalytic cycle at the microenvironment.
View Article and Find Full Text PDFJ Am Chem Soc
August 2025
Department of Chemistry and Biochemistry, The University of Texas at Dallas, Richardson, Texas 75080-3021, United States.
Halogen atom transfer (XAT) and single electron transfer (SET) have emerged as versatile tools for the generation of aryl radicals. The intrinsic reactivity of these methods is governed by bond dissociation energies (BDEs) and reduction potentials, respectively, which typically favor activation of an aryl iodide over an aryl bromide. To date, no existing methods have overturned these inherent reactivity trends.
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