A Promoted Charge Separation/Transfer System from Cu Single Atoms and C₃N₄ Layers for Efficient Photocatalysis

Advanced Materials, Год журнала: 2020, Номер 32(33)

Опубликована: Июль 9, 2020

Establishing highly effective charge transfer channels in carbon nitride (C3 N4 ) for enhancing its photocatalytic activity is still a challenging issue. Herein, the first time, engineering of C3 layers with single-atom Cu bonded compositional N (CuNx demonstrated to address this challenge. The CuNx formed by intercalation chlorophyll sodium copper salt into melamine-based supramolecular precursor followed controlled pyrolysis. Two groups are identified: one group each atoms three in-plane atoms, while other four two neighboring layers, thus forming both and interlayer channels. Importantly, ultrafast spectroscopy has further proved that can greatly improve separation/transfer carriers turn boost efficiency. Consequently, catalyst exhibits superior visible-light hydrogen production rate (≈212 µmol h-1 /0.02 g catalyst), 30 times higher than bulk . Moreover, it leads an outstanding conversion (92.3%) selectivity (99.9%) oxidation benzene under visible light.

Язык: Английский

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Updates on the Roadmap for Photocatalysis

ACS Catalysis, Год журнала: 2020, Номер 10(10), С. 5493 - 5501

Опубликована: Апрель 14, 2020

ADVERTISEMENT RETURN TO ISSUEPREVViewpointNEXTUpdates on the Roadmap for PhotocatalysisMichele MelchionnaMichele MelchionnaChemistry Department, INSTM and ICCOM-CNR Trieste Research Unit, University of Trieste, Via L. Giorgieri 1, 34127, ItalyMore by Michele Melchionnahttp://orcid.org/0000-0001-9813-9753 Paolo Fornasiero*Paolo FornasieroChemistry Italy*Email P.F.: [email protected]More Fornasierohttp://orcid.org/0000-0003-1082-9157Cite this: ACS Catal. 2020, 10, 5493–5501Publication Date (Web):April 14, 2020Publication History Received13 March 2020Published online14 April inissue 15 May 2020https://doi.org/10.1021/acscatal.0c01204Copyright © 2020 American Chemical SocietyRIGHTS & PERMISSIONSACS AuthorChoiceCC: Creative CommonsBY: Credit must be given to creatorArticle Views16419Altmetric-Citations196LEARN ABOUT THESE METRICSArticle Views are COUNTER-compliant sum full text article downloads since November 2008 (both PDF HTML) across all institutions individuals. These metrics regularly updated reflect usage leading up last few days.Citations number other articles citing this article, calculated Crossref daily. Find more information about citation counts.The Altmetric Attention Score is a quantitative measure attention that research has received online. Clicking donut icon will load page at altmetric.com with additional details score social media presence article. how calculated. Share Add toView InAdd Full Text ReferenceAdd Description ExportRISCitationCitation abstractCitation referencesMore Options onFacebookTwitterWechatLinked InReddit (4 MB) Get e-AlertsSUBJECTS:Catalysts,Materials,Metals,Photocatalysis,Photocatalysts e-Alerts

Язык: Английский

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New Redox Strategies in Organic Synthesis by Means of Electrochemistry and Photochemistry

ACS Central Science, Год журнала: 2020, Номер 6(8), С. 1317 - 1340

Опубликована: Июль 16, 2020

As the breadth of radical chemistry grows, new means to promote and regulate single-electron redox activities play increasingly important roles in driving modern synthetic innovation. In this regard, photochemistry electrochemistry-both considered as niche fields for decades-have seen an explosive renewal interest recent years gradually have become a cornerstone organic chemistry. Outlook article, we examine current state-of-the-art areas electrochemistry photochemistry, well nascent area electrophotochemistry. These techniques employ external stimuli activate molecules imbue privileged control reaction progress selectivity that is challenging traditional chemical methods. Thus, they provide alternative entries known reactive intermediates enable distinct strategies were previously unimaginable. Of many hallmarks, electro- are often classified "green" technologies, promoting reactions under mild conditions without necessity potent wasteful oxidants reductants. This reviews most growth these with special emphasis on conceptual advances given rise enhanced accessibility tools trade.

Язык: Английский

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Photocatalytic Late-Stage C–H Functionalization

Chemical Reviews, Год журнала: 2023, Номер 123(8), С. 4237 - 4352

Опубликована: Янв. 24, 2023

The emergence of modern photocatalysis, characterized by mildness and selectivity, has significantly spurred innovative late-stage C–H functionalization approaches that make use low energy photons as a controllable source. Compared to traditional strategies, photocatalysis paves the way toward complementary and/or previously unattainable regio- chemoselectivities. Merging compelling benefits with workflow offers potentially unmatched arsenal tackle drug development campaigns beyond. This Review highlights photocatalytic strategies small-molecule drugs, agrochemicals, natural products, classified according targeted bond newly formed one. Emphasis is devoted identifying, describing, comparing main mechanistic scenarios. draws critical comparison between established ionic chemistry photocatalyzed radical-based manifolds. aims establish current state-of-the-art illustrate key unsolved challenges be addressed in future. authors aim introduce general readership functionalization, specialist practitioners evaluation methodologies, potential for improvement, future uncharted directions.

Язык: Английский

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Visible light photocatalysis in the late-stage functionalization of pharmaceutically relevant compounds

Chemical Society Reviews, Год журнала: 2020, Номер 50(2), С. 766 - 897

Опубликована: Дек. 22, 2020

Recent developments and future prospects of visible-light photocatalysis in the late-stage functionalization pharmaceuticals natural bioactive compounds.

Язык: Английский

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Mechanistic analysis of multiple processes controlling solar-driven H2O2 synthesis using engineered polymeric carbon nitride

Nature Communications, Год журнала: 2021, Номер 12(1)

Опубликована: Июнь 17, 2021

Abstract Solar-driven hydrogen peroxide (H 2 O ) production presents unique merits of sustainability and environmental friendliness. Herein, efficient solar-driven H through dioxygen reduction is achieved by employing polymeric carbon nitride framework with sodium cyanaminate moiety, affording a rate 18.7 μmol h −1 mg an apparent quantum yield 27.6% at 380 nm. The overall photocatalytic transformation process systematically analyzed, some previously unknown structural features interactions are substantiated via experimental theoretical methods. cyanamino group pyridinic nitrogen-coordinated soidum in the promote photon absorption, alter energy landscape improve charge separation efficiency, enhance surface adsorption dioxygen, create selective 2e − oxygen reaction surface-active sites. Particularly, electronic coupling interaction between surface, which boosts population prolongs lifetime active shallow-trapped electrons, experimentally substantiated.

Язык: Английский

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Late-stage difluoromethylation: concepts, developments and perspective

Chemical Society Reviews, Год журнала: 2021, Номер 50(14), С. 8214 - 8247

Опубликована: Янв. 1, 2021

This review describes the conceptual advances that have led to multiple difluoromethylation processes making use of well-defined CF₂H sources.

Язык: Английский

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Unraveling fundamental active units in carbon nitride for photocatalytic oxidation reactions

Nature Communications, Год журнала: 2021, Номер 12(1)

Опубликована: Янв. 12, 2021

Covalently bonded carbon nitride (CN) has stimulated extensive attention as a metal-free semiconductor. However, because of the complexity polymeric structures, acquisition critical roles each molecular constituent in CN for photocatalysis remains elusive. Herein, we clarify fundamental active units by synthesizing with more detailed structures. Enabled microwave synthesis, as-prepared consists distinguishable melem (M1) and its incomplete condensed form (M2). We disclose rather than traditional opinion being involved whole photocatalytic processes, M1 M2 make primary contributions light absorption charge separation, respectively. Meanwhile, oxygen molecules are unusually observed to be activated participating photoexcited processes via electronic coupling mainly M2. As result, such higher activity, which was up 8 times that bulk oxidation tetracycline water.

Язык: Английский

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From isolated Ti-oxo clusters to infinite Ti-oxo chains and sheets: recent advances in photoactive Ti-based MOFs

Journal of Materials Chemistry A, Год журнала: 2020, Номер 8(31), С. 15245 - 15270

Опубликована: Янв. 1, 2020

This review highlights recent progress in Ti-MOFs based on discrete Ti-oxo clusters and infinite chains sheets.

Язык: Английский

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Heterogeneous Photocatalytic Organic Transformation Reactions Using Conjugated Polymers-Based Materials

ACS Catalysis, Год журнала: 2020, Номер 10(20), С. 12256 - 12283

Опубликована: Сен. 24, 2020

Photocatalytic heterogeneous organic transformation is considered as an efficient, clean atomic economy, and low-energy consumption strategy for synthesis. Conjugated polymers (CPs)-based materials have recently shown great potential diverse photocatalytic applications because of their unique properties, such structural designability, recyclability, high chemical stability, low cost, they emerged promising alternatives to traditional molecular or inorganic photocatalyst in photoredox reactions. Immense efforts been made toward the construction CPs-based versatile transformations. In this Review, we aim summarize recent progress photocatalysts transformations including oxidation, reduction, coupling, cycloaddition reaction. This Review discusses influence molecular, electronic, channel structure on light absorption, charge separation, mass transfer different The regulated synthesis, mechanistic discussions, future challenges systems are also considered. It expected that could not only deepen comprehension but open up inspirations feasibilities materials.

Язык: Английский

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