Photouranium-Catalyzed C–F Activation Hydroxylation via Water Splitting

Journal of the American Chemical Society, Journal Year: 2024, Volume and Issue: unknown

Published: April 9, 2024

The C–F bond is the strongest covalent single (126 kcal/mol) in carbon-centered bonds, which highest electronegativity of fluorine (χ = 4) gives rise to shortest length (1.38 Å) and smallest van der Waals radius (rw 1.47 Å), resulting enormous challenges for activation transformation. Herein, conversion was realized via photouranium-catalyzed hydroxylation unactivated aryl fluorides using water as a hydroxyl source deliver multifunctional phenols under ambient conditions. featured cascade sequences electron transfer (SET)/hydrogen atom (HAT)/oxygen (OAT), highly integrated from excited uranyl cation. *UO22+ prompted splitting mild photoexcitation, caging active oxygen peroxo-bridged manner critical OAT process releasing hydrogen HAT process.

Language: Английский

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Photochemical upcycling and recycling of plastics: achievements and future opportunities

Green Chemistry, Journal Year: 2024, Volume and Issue: 26(15), P. 8528 - 8549

Published: Jan. 1, 2024

Recent developments in the photochemical upcycling and recycling of plastics.

Language: Английский

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Catalytic recycling of plastics into value-added products

Nano Research, Journal Year: 2024, Volume and Issue: unknown

Published: Sept. 9, 2024

Language: Английский

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Coupling Plastic Upgrading and Photocatalysis: Catalytic Mechanisms and Design Principles

ACS Catalysis, Journal Year: 2025, Volume and Issue: unknown, P. 5339 - 5369

Published: March 17, 2025

Language: Английский

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Chemical Upcycling of Polyolefins through C−H Functionalization

European Journal of Organic Chemistry, Journal Year: 2023, Volume and Issue: 26(39)

Published: Aug. 9, 2023

Abstract Polyolefins consist of abundant hydrophobic C−C and C−H bonds, are considered as immensely potential untapped resources. Chemical upcycling offers a convenient promising recycling strategy polyolefins to produce newly‐functionalized polymeric materials, high‐value added chemicals. The significant progress made in functionalization reactions alkane molecules provides new opportunities for improving polyolefin treatments. This review focuses on recent advancements post‐modification routes, specifically the introduction C−X (X=O, N, S, halogens etc.) bonds onto chain backbones, well degradation models involving homogeneous functionalization. By emphasizing these developments, we aim highlight chemical enhancing treatment polyolefins.

Language: Английский

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Uranyl Photocatalyzed Polystyrene Oxidative Degradation under Visible Light in a Green Solvent

Industrial & Engineering Chemistry Research, Journal Year: 2024, Volume and Issue: 63(11), P. 4817 - 4824

Published: March 6, 2024

Polystyrene (PS) provides a huge convenience and promotes economic social development. However, difficulties in recycling degradation of PS make waste hazardous to the environment organisms. In recent years, up-recycling PS, which turns oxygenated monomer products with added value such as benzoic acid, has attracted much attention since it into treasure offers reference for pollution treatment. Considering solubility character solvent toxicity, volatility, explosiveness, herein, we described mild, green, effective under uranyl photocatalysis. The main high-value upgrading product, was obtained. Mechanism discussed based on multianalysis gas chromatography/mass spectrometry (GC-MS), gel permeation chromatography (GPC), infrared spectrum (IR), isotopic labeling, simulations small units, so on. addition, successful application 20-g scale sunlight demonstrated potential this method utilizing solar energy degradation.

Language: Английский

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Photocatalytic Upcycling and Depolymerization of Vinyl Polymers

Angewandte Chemie, Journal Year: 2024, Volume and Issue: 136(19)

Published: March 11, 2024

Abstract Photocatalytic upcycling and depolymerization of vinyl polymers have emerged as promising strategies to combat plastic pollution promote a circular economy. This mini review critically summarizes current developments in the degradation including polystyrene poly(meth)acrylates. Of these material classes, polymethacrylates possess unique possibility undergo photocatalytic back monomer under thermodynamically favourable conditions, thus presenting significant advantages over traditional thermal strategies. Our perspective on formidable challenges potential future directions are also discussed.

Language: Английский

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From aryl chlorides to phenols: Photouranium-catalyzed hydroxylation via water splitting

Chem Catalysis, Journal Year: 2024, Volume and Issue: 4(7), P. 101027 - 101027

Published: June 12, 2024

Language: Английский

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Deprotection of Benzyl-Derived Groups via Uranyl-Photocatalysis

Organometallics, Journal Year: 2024, Volume and Issue: 43(16), P. 1682 - 1686

Published: April 1, 2024

To circumvent the hazards associated with flammable/explosive hydrogen and address substrate compatibility issues in reductive systems, we developed a mild method for benzyl deprotection facilitated by uranium under visible light irradiation at ambient conditions. The uranium-oxo species, as metal-oxo-type photosensitizer, demonstrates moisture, enabling C–H activation through ligand-to-metal charge transfer (LMCT) excitation. Subsequent capture of radical atmospheric oxygen induces oxidation benzylic position. Removal semiacetal occurs, resulting C–O bond cleavage acidic This methodology, featuring conditions operational convenience, is compatible moisture oxygen. It presents complementary strategy synthesis pharmaceuticals organic materials.

Language: Английский

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Iron‐Catalyzed Oxidative Deconstruction of Polyethylene Terephthalate to Terephthalic Acid under O₂

Chinese Journal of Chemistry, Journal Year: 2024, Volume and Issue: 42(20), P. 2431 - 2437

Published: May 31, 2024

Comprehensive Summary It is urgent to recycle polyethylene terephthalate (PET) effectively, since it the most consumed synthetic polyester and its improper disposal has caused significant environmental pollution. The existing chemical recycling methods highly rely on nucleophilic substitutions hydrogenative depolymerizations, which typically require use of excess nucleophiles, strong acids or bases, expensive metal catalysts, explosive gas atmosphere. Here, we demonstrate a mild efficient protocol for oxidative depolymerization PET terephthalic acid using only an O 2 balloon. Terephthalic can be recycled from PET‐containing materials including series plastic products in daily life. employing relatively low loading iron complex, earth‐abundant transition metal, as catalyst preliminary results large‐scale reaction 38 g waste practical feasibility this degradation method. This method also applicable selective mixed plastics. work represents rare example demonstrates great potentials such concept recycling.

Language: Английский

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