Single Atom Embedding Enhanced Macroscopic Polarization in Carbon Nitride Nanosheets for pH-Universal Piezo-Photocatalytic Nitrate Reduction over a Wide Concentration Range

ACS Catalysis, Год журнала: 2025, Номер unknown, С. 4025 - 4038

Опубликована: Фев. 20, 2025

Язык: Английский

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Hidden Impurities Generate False Positives in Single Atom Catalyst Imaging

Angewandte Chemie International Edition, Год журнала: 2024, Номер 63(44)

Опубликована: Май 15, 2024

Single-atom catalysts (SACs) are an emerging class of materials, leveraging maximum atom utilization and distinctive structural electronic properties to bridge heterogeneous homogeneous catalysis. Direct imaging methods, such as aberration-corrected high-angle annular dark-field scanning transmission electron microscopy, commonly applied confirm the atomic dispersion active sites. However, interpretations data from these techniques can be challenging due simultaneous contributions intensity impurities introduced during synthesis processes, well any variation in position relative focal plane beam. To address this matter, paper presents a comprehensive study on two representative SACs containing isolated nickel or copper atoms. Spectroscopic techniques, including X-ray absorption spectroscopy, were employed prove high metal catalytic Employing microscopy combined with single-atom-sensitive energy loss we scrutinized thin specimens provide unambiguous chemical identification observed single-atom species thereby distinguish sites at level. Overall, underscores complexity characterization establishes importance use spectroscopy tandem resolution fully reliably characterize catalysts.

Язык: Английский

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A Guide to Chemical Reactions Design in Carbon Nitride Photocatalysis

ChemPhotoChem, Год журнала: 2024, Номер 8(4)

Опубликована: Янв. 5, 2024

Abstract Graphitic carbon nitride semiconductors are inexpensive and reusable photocatalysts, which actively studied in organic synthesis. Successful design of photocatalytic reactions is based on the next considerations. i) Thermodynamic feasibility photoinduced processes, involve transfer electrons or electron‐proton couples. ii) Redox activity reagents. iii) Reactivity open‐shell intermediates generated from Herein, we summarize current understanding how local chemical structure graphitic nitrides their redox potentials used to reactions. This work intends serve as a guideline for materials scientists, who willing apply involving substrates, chemists, interested dive into heterogeneous photocatalysis.

Язык: Английский

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Modulating Decarboxylative Oxidation Photocatalysis by Ligand Engineering of Atomically Precise Copper Nanoclusters

Journal of the American Chemical Society, Год журнала: 2024, Номер unknown

Опубликована: Сен. 19, 2024

Copper nanoclusters (Cu NCs) characterized by their well-defined electronic and optical properties are an ideal platform for organic photocatalysis exploring atomic-level behaviors. However, potential as greener, efficient catalysts challenging reactions like decarboxylative oxygenation under mild conditions remains unexplored. Herein, we present Cu

Язык: Английский

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Advancing Heterogeneous Organic Synthesis With Coordination Chemistry‐Empowered Single‐Atom Catalysts

Advanced Materials, Год журнала: 2024, Номер unknown

Опубликована: Сен. 18, 2024

Abstract For traditional metal complexes, intricate chemistry is required to acquire appropriate ligands for controlling the electron and steric hindrance of active centers. Comparatively, preparation single‐atom catalysts much easier with more straightforward effective accesses arrangement control The presence coordination atoms or neighboring functional on supports' surface ensures stability single‐atoms their interactions individual substantially regulate performance Therefore, collaborative interaction between surrounding environment enhances initiation reaction substrates formation transformation crucial intermediate compounds, which imparts significant catalytic efficacy, rendering them a valuable framework investigating correlation structure activity, as well mechanism in organic reactions. Herein, comprehensive overviews both homogeneous complexes reactions are provided. Additionally, reflective conjectures about advancement synthesis also proposed present reference later development.

Язык: Английский

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Photochemical Carbocatalysis: Fullerene‐, Carbon Nanotube‐ or Graphene‐Based Metal‐Free Photocatalysts for Organic Transformations

ChemCatChem, Год журнала: 2024, Номер 16(14)

Опубликована: Март 5, 2024

Abstract Synthetic photochemistry is a research field, where organic transformations are promoted by the presence of photoactive species, under light irradiation. In particular, sub‐field photoorganocatalysis, molecules used as photocatalysts, has been launched “green” and sustainable approach. Carbon allotrope nanostructures (CANs) their derivatives exhibit unique photophysical photochemical properties, which have exploited for preparation efficient metal‐free photocatalytic systems. This review summarizes progress on field carbocatalysis, presenting achievements fullerene‐, carbon nanotube‐ graphene‐based nanomaterials. Additionally, future prospects CAN‐based nanomaterials promoters also mentioned.

Язык: Английский

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Metal-free semiconductors for visible-light-induced carbocarboxylation of styrenes with aliphatic redox-active esters and CO₂

Green Chemistry, Год журнала: 2023, Номер 26(3), С. 1317 - 1321

Опубликована: Дек. 21, 2023

A metal-free heterogeneous photoredox system provides a mild, sustainable, and practical route for the carboxyalkylation of olefins using ambient carbon dioxide as C1 source aliphatic reactive esters building blocks.

Язык: Английский

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Graphitic Carbon Nitride as a Photocatalyst for Decarboxylative C(sp2)–C(sp3) Couplings via Nickel Catalysis

Angewandte Chemie International Edition, Год журнала: 2024, Номер unknown

Опубликована: Май 29, 2024

The development of robust and reliable methods for the construction C(sp

Язык: Английский

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Activation of Molecular Oxygen and Selective Oxidation with Metal Complexes

Accounts of Chemical Research, Год журнала: 2025, Номер unknown

Опубликована: Фев. 21, 2025

ConspectusSelective oxidation with molecular oxygen is one of the most appealing approaches to functionalization organic molecules and, yet at same time, challenging reactions facing synthesis due poor selectivity control. Molecular a green and inexpensive oxidant, producing water as only byproduct in oxidation. Not surprisingly, it has been used manufacturing many commodity chemicals industry. It also nature's choice oxidant drives variety critical life various other biologic processes. While past decades have witnessed great progress understanding, both structurally mechanistically, how nature exploits metalloenzymes, i.e., monooxygenases dioxygenases, tackle some reactions, e.g., methane methanol, there are small number well-defined, man-made metal complexes that reported enable selective compounds more relevant fine chemical pharmaceutical synthesis.In 10 years or so, our laboratories developed several transition shown they capable catalyzing under 1 atm O2. Thus, we an Fe(II)-bisimidazolidinyl-pyridine complex catalyzes oxygenation C–H bonds ethers concomitant release hydrogen gas instead water, when iron center replaced Fe(III), oxidative cleavage C═C olefins becomes feasible. To address low activity oxidizing less active olefins, Mn(II)-bipyridine complex, which aliphatic C–C diols, carboxyl units carboxylic acids visible light irradiation. Light necessary cleave off-cycle, inactive manganese dimer into catalytically Mn═O oxo species. Furthermore, found binuclear salicylate-bridged Cu(II) enables tetrahydroisoquinolines well bond cleavage, catalytic vitamin B1 analogue brought in, lactams takes place via carbene catalysis. Still further, readily accessible Rh(II)-terpyridine alcohols, being water-soluble, catalyst can be easily separated reused multiple times. In addition, recently unearthed simple protocol allows waste polystyrene depolymerized isolable, valuable chemicals. A cheap Brønsted acid acts catalyst, activating singlet state through complexation polymer irradiation, thereby depolymerizing polymer.

Язык: Английский

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g-C₃N₄-Based Heterogeneous Photocatalyzed Synthesis and Evaluation of Antitumor Activities of Fluoroalkylated 4H-Pyrido[1,2-a]pyrimidin-4-ones

The Journal of Organic Chemistry, Год журнала: 2025, Номер unknown

Опубликована: Фев. 26, 2025

The first example of heterogeneous photoredox-catalyzed fluoroalkylation 4H-pyrido[1,2-a]pyrimidin-4-ones has been developed. With low-cost commercial g-C3N4 as the recyclable photocatalyst and cheap sodium fluoroalkyl sulfonates source, a variety fluoroalkylated pyridopyrimidinones were constructed in moderate to high yields. present reaction can be easily scaled up with good efficiency, catalytic system reused 5 times slight loss activities. Furthermore, biological activity synthesized compounds was preliminarily investigated.

Язык: Английский

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