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Organometallic reagents are essential tools in both academic and industrial laboratories and the polarity separation within the carbon-metal bonds endows them with exceptional reactivities, but also imposes limitations, including air- and moisture-sensitivity, and flammability. Here, we demonstrate that stable and easily accessible benzylic (or allylic) boronate with alkali-metal alkoxide as the activator can act as reactive organometallic reagents. This strategy enables transition metal-free deprotonative C-H borylation of diverse (hetero)arenes. The polar organometallic nature of this process enables predictable and site-selective borylation by targeting the arenes's most acidic C-H bond. This approach can be coupled with Suzuki-Miyaura reaction to produce C-H arylation products. We have also applied this strategy to the dehalogenative borylation of aryl bromides and anionic polymerization of styrenes. Given the unique stability and structural diversity of organoboronates, their organometallic-type reactivities show promise as a powerful alternative to synthetic methodologies that rely on sensitive organometallic reagents.
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http://dx.doi.org/10.1038/s41467-025-60674-9 | DOI Listing |
Angew Chem Int Ed Engl
September 2025
State Key Laboratory of Physical Chemistry of Solid Surfaces, Key Laboratory of Chemical Biology of Fujian Province, and College of Chemistry and Chemical Engineering, Xiamen University, Xiamen, 361005, China.
The enantioselective construction of quaternary carbon stereocenters bearing amine functionalities represents a significant challenge in organic synthesis despite their prevalence in pharmaceutically active compounds. Herein, we report a versatile metallaphotoredox platform for the asymmetric incorporation of amine fragments onto quaternary carbons via coupling of alkene-tethered aryl bromides with readily available α-silylamines. This transformation proceeds under mild conditions without requiring organometallic reagents or stoichiometric reductants.
View Article and Find Full Text PDFOrg Lett
September 2025
Key Laboratory of Material Chemistry for Energy Conversion and Storage, Ministry of Education, Hubei Key Laboratory of Bioinorganic Chemistry and Materia Medica, School of Chemistry and Chemical Engineering, Huazhong University of Science and Technology (HUST), Wuhan 430074, P. R. China.
We report herein the first reductive alkylation/aldol reaction via dual nickel/photoredox catalysis. This catalytic strategy completes the traditional approaches that require the performance of reactive organometallic reagents. By the simple assembly of unactivated alkyl halides, α,β-unsaturated carbonyls, and aldehydes in one-pot reaction, a variety of synthetically valuable β-hydroxyl carbonyl compounds can be synthesized under mild conditions with moderate to good yields.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
September 2025
Department of Chemistry, Centre for Analysis and Synthesis (CAS), Lund University, Lund, 221 00, Sweden.
Due to their high reactivity, organolithium and organomagnesium addition to ketones is usually performed under inert atmosphere at low temperature. Recent work has shown that, by dissolving the substrate in deep eutectic solvents (DES), these processes can be carried out on the benchtop, in air at room temperature. Surprisingly, the organometallic reagent, added to the DES from an organic solution, works in these conditions and gives better yields than in the standard setup.
View Article and Find Full Text PDFAcc Chem Res
September 2025
Department of Chemistry, Fudan University, Shanghai 200433, China.
ConspectusThe past decade has witnessed rapid growth in the synthesis of main-group element clusters, driven by advances in the design of Zintl phase precursors and their integration with organometallic reagents. These strategies have unlocked unprecedented structural motifs and bonding patterns, greatly enriching the landscape of main-group cluster chemistry. Among them, antimony-based clusters stand out for their diverse architectures and unique electronic properties, serving as ideal models to explore metalloid aromaticity, multicenter bonding, and unconventional Sb-Sb or Sb-metal interactions.
View Article and Find Full Text PDFOrganometallics
June 2025
Department of Chemistry, University of Michigan, Ann Arbor, Michigan 48104, United States.
This article describes a detailed investigation of the palladium-catalyzed coupling of aryl (pseudo)halides (ArX) with MSCF to form aryl trifluoromethylthioethers (ArSCF). Mechanistic organometallic studies are used to interrogate two key elementary steps of the catalytic cycle: (1) transmetalation of Pd(Ar)(X) complexes with MSCF and (2) Ar-SCF bond-forming reductive elimination. These studies reveal that tetramethylammonium trifluoromethylthiolate, NMeSCF, exhibits a combination of fast kinetics and high chemoselectivity for transmetalation.
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