Visible-light photocatalytic di- and hydro-carboxylation of unactivated alkenes with CO2

Nature Catalysis, Journal Year: 2022, Volume and Issue: 5(9), P. 832 - 838

Published: Sept. 15, 2022

Language: Английский

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Visible‐to‐UV Photon Upconversion: Recent Progress in New Materials and Applications

Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 62(25)

Published: March 8, 2023

Ultraviolet (UV, λ<400 nm) light is essential for various photochemical reactions, but its intensity in the solar spectrum very low, and sources that artificially generate high-energy UV are inefficient environmentally unfriendly. A solution to this problem photon upconversion (UC) from visible (vis, λ>400 light. Among several mechanisms, UC based on triplet-triplet annihilation (TTA-UC) particular has made remarkable progress recent years. The development of new chromophores enabled highly efficient conversion low-intensity into In review, we summarize visible-to-UV TTA-UC, their production films application processes such as catalysis, bond activation polymerization. Finally, challenges opportunities future material applications will be discussed.

Language: Английский

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Challenges and Future Perspectives in Photocatalysis: Conclusions from an Interdisciplinary Workshop

JACS Au, Journal Year: 2024, Volume and Issue: 4(8), P. 2746 - 2766

Published: Aug. 8, 2024

Photocatalysis is a versatile and rapidly developing field with applications spanning artificial photosynthesis, photo-biocatalysis, photoredox catalysis in solution or supramolecular structures, utilization of abundant metals organocatalysts, sustainable synthesis, plastic degradation. In this Perspective, we summarize conclusions from an interdisciplinary workshop young principal investigators held at the Lorentz Center Leiden March 2023. We explore how diverse fields within photocatalysis can benefit one another. delve into intricate interplay between these subdisciplines, by highlighting unique challenges opportunities presented each multidisciplinary approach drive innovation lead to solutions for future. Advanced collaboration knowledge exchange across domains further enhance potential photocatalysis. Artificial photosynthesis has become promising technology solar fuel generation, instance, via water splitting CO

Language: Английский

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Photocatalyzed Cascade Reactions of Cyclopropanols and α‐Trifluoromethyl‐Substituted Olefins for the Synthesis of Fused gem‐Difluorooxetanes

Angewandte Chemie International Edition, Journal Year: 2022, Volume and Issue: 61(44)

Published: Sept. 16, 2022

Fluorinated fused rings are challenging to construct from simple starting materials. Herein, we report the first photocatalyzed cascade reactions of readily available cyclopropanols and α-trifluoromethyl-substituted olefins for synthesis gem-difluorooxetanes. Two three bonds were efficiently constructed in one reaction. The reaction showed broad substrate scope downstream transformations products demonstrated synthetic potential mechanistic study supported presence photoredox catalysis energy transfer catalysis/direct photo-excitation processes.

Language: Английский

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Blue‐to‐UVB Upconversion, Solvent Sensitization and Challenging Bond Activation Enabled by a Benzene‐Based Annihilator

Angewandte Chemie International Edition, Journal Year: 2022, Volume and Issue: 62(8)

Published: Nov. 18, 2022

Several energy-demanding photoreactions require harsh UV light from inefficient sources. The conversion of low-energy visible to high-energy singlet states via triplet-triplet annihilation upconversion (TTA-UC) could offer a solution for driving such reactions under mild conditions. We present the first annihilator with an emission maximum in UVB region that, combined organic sensitizer, is suitable blue-to-UVB upconversion. was successfully employed as energy donor subsequent FRET activations aliphatic carbonyls. This hitherto unreported UC-FRET reaction sequence directly monitored using laser spectroscopy and applied mechanistic irradiation experiments demonstrating feasibility Norrish chemistry. Our results provide clear evidence novel blue light-driven substrate or solvent activation strategy, which important context developing more sustainable light-to-chemical systems.

Language: Английский

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Red light-driven electron sacrificial agents-free photoreduction of inert aryl halides via triplet-triplet annihilation

Nature Communications, Journal Year: 2023, Volume and Issue: 14(1)

Published: Feb. 27, 2023

Selective photoactivation of inert aryl halides is a fundamental challenge in organic synthesis. Specially, the long-wavelength red light more desirable than widely-applied blue as excitation source for photoredox catalysis, due to its superior penetration depth. However, light-driven remains challenge, mainly because low energy single photon. Herein, we report photoreduction bromides/chlorides with 656 nm LED via triplet-triplet annihilation (TTA) strategy. This method based on our discovery that commonly used chromophore perylene can serve an efficient and metal-free photocatalyst enable without conventional need electronic sacrificial agents. By introducing light-absorbing photosensitizer this system, accomplish sensitized TTA mechanism. Moreover, performance such TTA-mediated be significantly enhanced when restricting rotation freedom phenyl moiety derivatives suppress their triplet nonradiative transition, both small large-scale reaction settings.

Language: Английский

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Bimodal Electrochemiluminescence Microscopy of Single Cells

Analytical Chemistry, Journal Year: 2023, Volume and Issue: 95(18), P. 7372 - 7378

Published: April 25, 2023

Electrochemiluminescence (ECL) microscopy is an emerging technique with new applications such as imaging of single entities and cells. Herein, we have developed a bimodal bicolor approach to record both positive ECL (PECL: light-emitting object on dark background) shadow label-free (SECL: nonemissive shadowing the background luminescence) images This result simultaneous emissions [Ru(bpy)3]2+ used label cellular membrane (PECL) [Ir(sppy)3]3– dissolved in solution (SECL). By spectrally resolving emission wavelengths, recorded same cells PECL SECL modes using (λmax = 620 nm) 515 luminescence, respectively. shows distribution labels attached membrane, whereas reflects local diffusional hindrance reagents by each cell. The high sensitivity surface-confined features reported are demonstrated cell–cell contacts during mitosis process. Furthermore, comparison demonstrates differential diffusion tri-n-propylamine through permeabilized cell membranes. Consequently, this dual enables morphology adhering surface can significantly contribute multimodal bioassays different luminescent systems.

Language: Английский

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A visible-light-promoted metal-free approach for N–H insertions by using donor/donor diazo precursors

Green Chemistry, Journal Year: 2024, Volume and Issue: 26(8), P. 4600 - 4608

Published: Jan. 1, 2024

A metal-free and catalyst-free strategy is reported to achieve N–H insertions by coupling N -tosylhydrazones with diverse amines including aminopyridines, anilines, aliphatic amines, other nucleophiles such as imidazoles indoles.

Language: Английский

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Redox mediated enhancement and quenching of co-reactant electrochemiluminescence by iridium(III) complexes

Electrochimica Acta, Journal Year: 2024, Volume and Issue: 484, P. 143957 - 143957

Published: Feb. 14, 2024

Enhancement of the electrochemiluminescence (ECL) tris(2,2′-bipyridine)ruthenium(II) ([Ru(bpy)3]2+) and tri-n-propylamine by redox mediators has emerged as a new approach to maximise sensitivity this mode detection. Herein, we examine influence six water-soluble iridium(III) complexes on widely used ECL system deconvoluting their respective contributions overall intensity over range applied potentials. The interconnected co-reactant these metal complexes, eliciting enhancement or quenching [Ru(bpy)3]2+ emission, can be understood considering available reaction pathways under different conditions disparate electrochemical photophysical properties reactants. ideal for are established, which will inform future design application in system.

Language: Английский

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Aggregation-Induced Emission Luminogens for Latent Fingerprint Detection

Chemical Communications, Journal Year: 2024, Volume and Issue: 60(64), P. 8314 - 8338

Published: Jan. 1, 2024

For over a century, fingerprints have served as pivotal tool for identification of individuals owing to their enduring characteristics and easily apparent features, particularly in the realm criminal investigations. Latent (LFPs) are "invisible fingerprints" that most commonly available at crime scenes require rapid, selective, sensitive, convenient method detection. However, existing fingerprint development techniques harbour limitations, prompting exploration novel approaches prioritize investigator safety environmental sustainability. Leveraging unique photophysical properties aggregation-induced emission luminogens (AIEgens) has emerged promising strategy on-site analysis LFP visualization. In this highlight, we presented comparative various AIEgens (organic compounds, metal complexes, nanoparticles, polymers) detection LFPs. Through examination, insights into efficiency potential applications AIE-based provided. addition, several strategies been proposed circumventing limitations AIEgens. We hope highlight article will encourage more researchers investigate detection, contributing forensic science.

Language: Английский

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