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Modular assembly of amines and diborons with photocatalysis enabled halogen atom transfer of organohalides for C(sp)-C(sp) bond formation.
Chem Sci
January 2025
College of Chemistry and Chemical Engineering, Key (Guangdong-Hong Kong Joint) Laboratory for Preparation and Application of Ordered Structural Materials of Guangdong Province, Shantou University Shantou 515063 P. R. China
In the past few years, the direct activation of organohalides by ligated boryl radicals has emerged as a potential synthetic tool for cross-coupling reactions. In most existing methods, ligated boryl radicals are accessed from NHC-boranes or amine-boranes. In this work, we report a new photocatalytic platform by modular assembly of readily available amines and diboron esters to access a library of ligated boryl radicals for reaction screening, thus enabling the cross-coupling of organohalides and alkenes including both activated and unactivated ones for C(sp)-C(sp) bond formation by using the assembly of DABCO A1 and BNepB1.
View Article and Find Full Text PDFChemical upcycling of polybutadiene into size controlled α,ω-dienes and diesters sequential hydrogenation and cross-metathesis.
Chem Sci
January 2025
Centre for Membrane Separations, Adsorption, Catalysis and Spectroscopy for Sustainable Solutions (cMACS), KU Leuven Celestijnenlaan 200F, Post Box 2454 3001 Leuven Belgium
Plastic waste conversion into valuable chemicals is a promising alternative to landfill or incineration. In particular, the chemical upcycling of polybutadiene rubber (PBR) could provide a renewable route towards highly desirable α,ω-dienes with varying chain lengths, which can find ample industrial application. While previous research has shown that the treatment of polybutadiene with a consecutive hydrogenation and ethenolysis reaction can afford long-chain α,ω-dienes, achieving precise control over the product chain length remains an important bottleneck.
View Article and Find Full Text PDFLanthanide-tetrazine probes for bio-imaging and click chemistry.
Chem Sci
January 2025
Department of Chemistry, Imperial College London Molecular Sciences Research Hub, 82 Wood Lane, White City Campus London W12 0BZ UK
The blood-brain-barrier prevents many imaging agents and therapeutics from being delivered to the brain that could fight central nervous system diseases such as Alzheimer's disease and strokes. However, techniques such as the use of stapled peptides or peptide shuttles may allow payloads through, with bioconjugation achieved bio-orthogonal tetrazine/norbornene click chemistry. A series of lanthanide-tetrazine probes have been synthesised herein which could be utilised in bio-orthogonal click chemistry with peptide-based delivery systems to deliver MRI agents through the blood-brain-barrier.
View Article and Find Full Text PDFPolarity reversal, or "umpolung", is a widely acknowledged strategy to allow organic functional groups amenable to react in alternative ways to the usual preference set by their electronic features. In this article, we demonstrate that cyclohexyne umpolung, realized through complexation to zirconocene, makes the small strained cycloalkyne amenable to C-F bond functionalisation. Such strong bond activation chemistry is unprecedented in "free" aryne and strained alkyne chemistry.
View Article and Find Full Text PDFLigand-induced changes in the electrocatalytic activity of atomically precise Au nanoclusters.
Chem Sci
January 2025
School of Chemistry and Chemical Engineering, Chongqing Key Laboratory of Chemical Theory and Mechanism, Chongqing University Chongqing 401331 China
Atomically precise gold nanoclusters have shown great promise as model electrocatalysts in pivotal electrocatalytic processes such as the hydrogen evolution reaction (HER) and carbon dioxide reduction reaction (CORR). Although the influence of ligands on the electronic properties of these nanoclusters is well acknowledged, the ligand effects on their electrocatalytic performances have been rarely explored. Herein, using [Au(SR)] nanoclusters as a prototype model, we demonstrated the importance of ligand hydrophilicity hydrophobicity in modulating the interface dynamics and electrocatalytic performance.
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