Molecular Carbon Imides

Journal of the American Chemical Society, Journal Year: 2022, Volume and Issue: 144(33), P. 14976 - 14991

Published: July 29, 2022

The creation and development of new forms nanocarbons have fundamentally transformed the scientific landscape in past three decades. As members nanocarbon family with accurate size, shape, edge structure, molecular carbon imides (MCIs) shown unexpected unique properties. Particularly, imide functionalization strategy has endowed these rylene-based carbons fascinating characteristics involving flexible syntheses, tailor-made structures, diverse properties, excellent processability, good stability. This Perspective elaborates design evolution to functional landscapes, illustrative examples are given, including a promising library multi-size multi-dimensional MCIs rigidly conjugated π-architectures, ranging from 1D nanoribbon 2D nanographene cross-dimensional MCIs. Although researchers achieved substantial progress using as components for exploration charge transport, photoelectric conversion, chiral luminescence performances, they far unleashing their full potential. Developing highly efficient regioselective coupling/ring-closure reactions formation multiple C–C bonds annulation electron-deficient aromatic units is crucial. Prediction by theory help machine learning artificial intelligence research along reliable nanotechnology characterization will give an impetus blossom related fields. Future investigations also advance toward─or even focus on─the emerging potential functions, especially fields electronics spin electronics, which expected open avenues.

Language: Английский

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Helical Synthetic Nanographenes with Atomic Precision

Accounts of Chemical Research, Journal Year: 2023, Volume and Issue: 56(3), P. 363 - 373

Published: Jan. 26, 2023

ConspectusUnderstanding and harnessing the properties of nanoscale molecular entities are considered as new frontiers in basic chemistry. In this regard, synthetic nanographene with atomic precision has attracted much attention recently. For instance, taking advantage marvelous bonding capability carbon, flat, curved, ribbon-type, or cone-shaped nanographenes have been prepared highly controllable elegant manner, allowing one to explore fascinating architectures intriguing optical, electrochemical, magnetic characteristics. This stands stark contrast other carbon-rich nanomaterials, such graphite oxides carbon quantum dots, which preclude thorough investigations because complicate structural defects. Undoubtedly, contributes strongly modern aromatic chemistry represents a vibrant field that may deliver transforming functional materials crucial for optoelectronics, nanotechnologies, biomedicine.Nonetheless, many cases, synthesis characterization compounds demanding. Low solubility, high strain, undesired selectivity, well incomplete excessive C-C bond formation common impediments, require formidable efforts control geometry, modulate edge structure, achieve accurate doping, push upper size boundary. These endeavors indispensable establishing structure-property relationships, lay down foundation exploring at level sophistications.In Account, we summarize our contributions by presenting series helical nanographenes, hexapole [7]helicene (H7H), nitrogen-doped H7H, [9]helicene (H9H), superhelicene, supertwistacene. kind giant reaches domain albeit precise structure. It provides unique platform study chirality nanoscale. We discuss methods point out, particular, strengths pitfalls Scholl oxidation, expected be valuable making general. addition, illustrate their exciting electrochemical photophysical performance, include, but not limited to, reversible multielectron redox chemistry, record panchromatic absorption, impressive photothermal behavior, extremely strong Cotton effect. unusual characteristics convincingly traced back three-dimensional conjugated architectures, highlighting critical roles π-electron delocalization, heteroatom-doping, substitution, symmetry determining nanographenes' functions. Lastly, put forward understanding on challenges opportunities lies ahead hope Account will inspire ever more ambitious achievements from attractive area research.

Language: Английский

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Onion-like multicolor thermally activated delayed fluorescent carbon quantum dots for efficient electroluminescent light-emitting diodes

Nature Communications, Journal Year: 2024, Volume and Issue: 15(1)

Published: April 8, 2024

Abstract Carbon quantum dots are emerging as promising nanomaterials for next-generation displays. The elaborate structural design is crucial achieving thermally activated delayed fluorescence, particularly improving external efficiency of electroluminescent light-emitting diodes. Here, we report the synthesis onion-like multicolor fluorescence carbon with yields 42.3–61.0%. Structural, spectroscopic characterization and computational studies reveal that structures assembled from monomer different sizes account decreased singlet-triplet energy gap, thereby efficient fluorescence. devices exhibit maximum luminances 3785–7550 cd m −2 6.0–9.9%. Importantly, owing to weak van der Waals interactions adequate solution processability, flexible a luminance 2554 realized. These findings facilitate development high-performance dots-based diodes practical applications.

Language: Английский

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Synthesis of monolayer and persistent bilayer graphene fragments by using a radical-mediated coupling approach

Nature Synthesis, Journal Year: 2023, Volume and Issue: 2(11), P. 1104 - 1115

Published: June 15, 2023

Language: Английский

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Preferential molecular recognition of heterochiral guests within a cyclophane receptor

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

Published: Jan. 16, 2023

The discrimination of enantiomers by natural receptors is a well-established phenomenon. In contrast the number synthetic with capability for enantioselective molecular recognition chiral substrates scarce and cyclophanes indicative preferential binding homochiral guests. Here we introduce cyclophane composed two core-twisted perylene bisimide (PBI) units connected p-xylylene spacers demonstrate its preference complexation [5]helicene opposite helicity compared to PBI host. pronounced enantio-differentiation this receptor heterochiral guests can be utilized enrichment P-PBI-M-helicene-P-PBI epimeric bimolecular complex. Our experimental results are supported DFT calculations, which reveal that sterically demanding bay substituents attached chromophores disturb helical shape match core thereby enforce formation syndiotactic host-guest complex structures. Hence, most efficient substrate observed those aromatic guests, e. g. perylene, [4]helicene, phenanthrene biphenyl, easily adapt in non-planar axially conformations due their inherent conformational flexibility. all cases induced chirality guest opposed embedding units, leading

Language: Английский

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Helical Trilayer Nanographenes with Tunable Interlayer Overlaps

Journal of the American Chemical Society, Journal Year: 2023, Volume and Issue: 145(5), P. 2815 - 2821

Published: Jan. 27, 2023

The synthesis of well-defined nanocarbon multilayers, beyond the bilayer structure, is still a challenging goal. Herein, two trilayer nanographenes were synthesized by covalently linking nanographene layers through helicene bridges. structural characterization revealed compact trilayer-stacked architecture. introduction furan ring into linker modulates interlayer overlap and π-conjugation nanographenes, enabling tuning coupling, as demonstrated optical, electrochemical, theoretical analyses. Both are rigid chiral nanocarbons show chirality transfer from moiety to stacked layers. These helical reported here represent linked multilayer rather than ones, showing tunable stacking structure.

Language: Английский

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Engineering Soluble Diketopyrrolopyrrole Chromophore Stacks from a Series of Pd(II)‐Based Ravels**

Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 62(40)

Published: July 17, 2023

Abstract A strategy to engineer the stacking of diketopyrrolopyrrole (DPP) dyes based on non‐statistical metallosupramolecular self‐assembly is introduced. For this, DPP backbone equipped with nitrogen‐based donors that allow for different discrete assemblies be formed upon addition Pd(II), distinguished by number π‐stacked chromophores. Pd 3 L 6 three‐ring, a heteroleptic 2 L′ ravel composed two crossing DPPs (flanked carbazoles), and unprecedented self‐penetrated motifs (a triple 4 quadruple stack), were obtained systematically investigated. With increasing counts stacked chromophores, UV/Vis absorptions red‐shift emission intensities decrease, except compound , which stands out an exceptional photoluminescence quantum yield 51 %. This extraordinary open‐shell metal containing explainable intra‐assembly FRET process. The modular design synthesis soluble multi‐chromophore building blocks offers potential preparation nanodevices materials applications in sensing, photo‐redox catalysis optics.

Language: Английский

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Overview of the impact of oxygenated biofuel additives on soot emissions in laboratory scale

Fuel Processing Technology, Journal Year: 2024, Volume and Issue: 254, P. 108046 - 108046

Published: Jan. 30, 2024

Soot has harmful effects on the environment and human health. The formation process of soot includes six steps: fuel pyrolysis, nucleation, coalescence, surface growth, aggregation, oxidation. However, is very complex influenced by factors such as type, combustion conditions, environmental temperature. Oxygenated fuels additives have a positive effect reducing emissions, but recent studies shown that oxygenated can lead to an increase in number small particles soot. In this paper, alcohol, ether, esters emissions discussed terms mechanism formation. Subsequently, role after-treatment systems summarized. This work update our understanding impact emissions.

Language: Английский

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Novel hydrogen-bonded organic framework (HOF) for highly efficient photocatalysis: From structural designs to multifunctional applications

Coordination Chemistry Reviews, Journal Year: 2025, Volume and Issue: 535, P. 216634 - 216634

Published: March 20, 2025

Language: Английский

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Mimicking DNA Periodic Docking Grooves for Adaptive Identification of l-/d-Tryptophan in a Biological Metal–Organic Framework

Journal of the American Chemical Society, Journal Year: 2022, Volume and Issue: 144(22), P. 9559 - 9563

Published: May 23, 2022

Bioinspired metal–organic frameworks (MOFs) serve as suitable crystalline models for recognition and sensing of biomolecules mimicking natural processes, providing new ideas concepts cutting-edge biomedical applications. Here, we have successfully prepared a robust biological framework with periodic docking grooves resembling the major minor in DNA double helix structure, which can be used unique sites selectively identifying l-/d-tryptophan (l-/d-Trp). Notably, successful encapsulation Trp could observed by single-crystal X-ray diffraction first time. has matched size shape to fit snugly into groove. Combined isothermal titration calorimetry, it was found that ZnBTCHx spontaneously capture l-/d-Trp through two different thermodynamic pathways: enthalpy-driven encapsulating l-Trp entropy-driven uptaking d-Trp. Furthermore, molecular dynamics density functional theory verified role hydrogen bonding π–π/C–H···π interactions host–guest interface. This work provides insight construction bionic mimic binding properties, is great significance fields pharmaceutical chemistry science.

Language: Английский

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