Defying the oxidative-addition prerequisite in cross-coupling through artful single-atom catalysts

Research Square (Research Square), Journal Year: 2025, Volume and Issue: unknown

Published: March 25, 2025

Heterogeneous single-atom catalysts (SACs) have gained significant attention for their maximized atom utilization and well-defined active sites, but they often struggle with multi-stage organic cross-coupling reactions due to limited coordination space reactivity. Here, we report an “anchoring-borrowing” strategy combined facet engineering develop artful (ASACs) through anchoring foreign single atoms onto specific facets of the non-innocent reducible carriers. ASACs exhibit adaptive coordination, effectively bypassing oxidative-addition prerequisite bivalent elevation at a metal site in both homogenous heterogeneous cross-couplings. For example, Pd₁-CeO₂(110) ASAC exhibits unparalleled activity coupling more accessible aryl chlorides, challenging heterocycles, outperforming traditional remarkable turnover number 45,327,037. Mechanistic studies reveal that leverage dynamic structural changes, carriers acting as electron reservoirs, significantly lowering reaction barriers. Furthermore, enable efficient synthesis biologically compounds, drug intermediates, pharmaceutical ingredients (APIs) scalable high-speed circulated flow synthesis, underscoring great potential sustainable fine chemical manufacturing.

Language: Английский

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Copper catalyzed carbon-selenium bond formation via the coupling reaction of aryl halides, phenylboronic acid and Se

Scientific Reports, Journal Year: 2025, Volume and Issue: 15(1)

Published: April 16, 2025

This is the first report for C-Se bond formation involving reaction of aryl halides with arylboronic acid and selenium powder to synthesis unsymmetrical diaryl selenides in presence CuI as a homogeneous catalyst. A wide range react various substituted groups under optimal conditions provide desired good high yields. Also, same reactions were investigated M-MCF@Gua-Cu reusable magnetic nanocatalyst conditions. The catalyst allows simpler (easy work-up) greener methodology. In addition, advantages presented method include use acid/Se safe cost-effective arylselenating system, simplicity operation, green cheap solvent.

Language: Английский

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Modern organic transformations: heterogeneous thermocatalysis or photocatalysis?

Chemical Society Reviews, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 1, 2025

This review presents the working principles, advantages and disadvantages of heterogeneous thermo- photocatalysis in organic transformations, outlines related applications advancements photocatalytic transformations.

Language: Английский

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Simultaneous Generation of Methyl Esters and CO in Lignin Transformation

Angewandte Chemie International Edition, Journal Year: 2022, Volume and Issue: 61(40)

Published: Aug. 18, 2022

Lignin is an abundant renewable carbon source. Due to its complex structure, utilization of lignin very challenging. Herein, we describe efficient strategy for the simultaneous lignin, in which methoxy groups react with carboxylic acids generate methyl carboxylates and other alkyl phenyl carbons oxygen predominantly form CO that can be used directly carbonylation reactions. The method was applied methylation various functionalized aryl acids, including natural compounds, produce valuable chemicals, pharmaceuticals. No solid or liquid residues remain after reaction. Mechanistic studies demonstrate a well-ordered C-C C-O bond activation sequence takes place realize total transformation lignin. This work opens way entire polymer into products, exemplified by synthesis pharmaceutical, Ramipril, on gram scale.

Language: Английский

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Recent advancements review Suzuki and Heck reactions catalyzed by metalloporphyrins

Inorganic Chemistry Communications, Journal Year: 2022, Volume and Issue: 149, P. 110359 - 110359

Published: Dec. 30, 2022

Language: Английский

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