Cu–N interface electron channel and photothermal synergistic catalysis enable more efficient selective oxidation of benzylamine to N-benzylidenebutylamine

Applied Surface Science, Journal Year: 2025, Volume and Issue: 688, P. 162331 - 162331

Published: Jan. 8, 2025

Language: Английский

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Diketopyrrolopyrrole‐based Donor–Acceptor Covalent Organic Frameworks for Iodine Capture

Small, Journal Year: 2025, Volume and Issue: unknown

Published: March 5, 2025

The recovery of radioactive iodine from nuclear waste and contaminated water sources is a critical environmental concern, which poses significant technical challenges. Herein, the study has demonstrated that tuning electronic properties diketopyrrolopyrrole-based donor-acceptor covalent organic frameworks (COFs) enhances trapping, improves charge transport, strengthens interactions - establishing structure-property relationship. This achieved by synthesizing COFs with linker 3,6-bis(4-(1,3-dioxolan-2-yl)phenyl)-2,5-dihydropyrrolo[3,4-c]pyrrole-1,4-dione (DKP) in combination either electron acceptor 4,4',4″-(1,3,5-triazine-2,4,6-triyl)trianiline (TTT-DKP) or donor N1,N1-bis(4-aminophenyl)benzene-1,4-diamine (TAPA-DKP) linkers. These COFs, abundant sorption sites, thermal chemical stability, optimized pore environments, efficiently bind vapor solution phases. TAPA-DKP COF, containing electron-donating moieties, showed high uptake 3.52 g/g, exceeding 2.81 g/g electron-deficient TTT-DKP phase, both following pseudo-second-order kinetics. Density functional theory (DFT) calculations reveal adsorption sites showing COF binds I2 more effectively via its electron-rich highlighting role property modulation adsorption.

Language: Английский

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Diketopyrrolopyrrole-triggered low exciton binding energy in D-A covalent organic framework for enhanced uranyl photoreduction

Separation and Purification Technology, Journal Year: 2024, Volume and Issue: 359, P. 130376 - 130376

Published: Nov. 12, 2024

Language: Английский

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Diketopyrrolopyrrole‐Activated Dynamic Condensation Approach to Narrow‐Band Gap Vinylene‐Linked Covalent Organic Frameworks

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: unknown

Published: Nov. 12, 2024

Vinyl units intrinsically featuring less steric, nonpolarity, and unsaturated character, are well-known π-bridge used in the synthesis of high-performance semiconducting materials. Two-dimensional (2D) vinylene-linked covalent organic frameworks (COFs) represent a promising class π-conjugated structures, however, range available monomers for reversible formation carbon-carbon double bonds remains limited. In this study, new 2D COFs were synthesized using dimethyldiketopyrrolopyrrole (DM-DPP) as key monomer. The strong electron deficiency diketopyrrolopyrrole (DPP) makes its methyl substituents readily activated upon cocatalysis L-proline 4-dimethylaminopyridine aqueous solution to conduct dynamic condensation with tritopic aromatic aldehydes. resulting crystallized an eclipsed AA stacking arrangement featured abundant, regular nanochannels. Their robust vinyl DPP-linking mode enhanced donor-π-acceptor conjugation promoted π-stacked alignment along vertical direction. Consequently, exhibited band gaps narrow 1.02 eV demonstrated excellent light-harvesting capability across visible near-infrared I (NIR-I) regions. Furthermore, could be converted into free-standing thin pellets through simple pressure casting, show photothermal response cycling stability under different light sources.

Language: Английский

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Tuning (Photo)Electronic Properties of an Electron Deficient Porous Polymer via n‐Doping with Tetrathiafulvalene

Small, Journal Year: 2024, Volume and Issue: unknown

Published: Aug. 29, 2024

Charge-transfer complex formation within the pores of porous polymers is an efficient way to tune their electronical properties. Introduction electron accepting guests donating hosts conduct p-doping intensively studied in this context. However, vice versa scenario, n-doping by treating deficient (i.e., n-type) with dopants, rare. In work, synthesis n-type phenazine based conjugated microporous polymer and its exposure strong tetrathiafulvalene (TTF) dopants are presented. The fundamental physical characterizations (e.g., elemental analysis, gas sorption) showed that vacuum impregnation technique a good approach load guest molecules inside pores. Moreover, charge-transfer complexes between building blocks polymeric network TTF confirmed via spectral techniques such Fourier transform infra-red, UV-vis, steady-state/time-resolved photoluminescence, transient absorbance spectroscopies. Effect doping properties monitored employing photoelectrochemical measurements, which lower resistivity nearly doubled photocurrents after doping. study is, therefore, important advancement for applicability (n-type) materials field photo(electro)catalysis organic electronics.

Language: Английский

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Diketopyrrolopyrrole‐Activated Dynamic Condensation Approach to Narrow‐Band Gap Vinylene‐Linked Covalent Organic Frameworks

Angewandte Chemie, Journal Year: 2024, Volume and Issue: unknown

Published: Nov. 12, 2024

Abstract Vinyl units intrinsically featuring less steric, nonpolarity, and unsaturated character, are well‐known π‐bridge used in the synthesis of high‐performance semiconducting materials. Two‐dimensional (2D) vinylene‐linked covalent organic frameworks (COFs) represent a promising class π‐conjugated structures, however, range available monomers for reversible formation carbon‐carbon double bonds remains limited. In this study, new 2D COFs were synthesized using dimethyldiketopyrrolopyrrole (DM‐DPP) as key monomer. The strong electron deficiency diketopyrrolopyrrole (DPP) makes its methyl substituents readily activated upon cocatalysis L‐proline 4‐dimethylaminopyridine aqueous solution to conduct dynamic condensation with tritopic aromatic aldehydes. resulting crystallized an eclipsed AA stacking arrangement featured abundant, regular nanochannels. Their robust vinyl DPP‐linking mode enhanced donor‐π‐acceptor conjugation promoted π‐stacked alignment along vertical direction. Consequently, exhibited band gaps narrow 1.02 eV demonstrated excellent light‐harvesting capability across visible near‐infrared I (NIR‐I) regions. Furthermore, could be converted into free‐standing thin pellets through simple pressure casting, show photothermal response cycling stability under different light sources.

Language: Английский

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Near-IR absorbing Tetraene-linked π-Conjugated Porous Polymer for Energy Storage and Electrical Conductivity

Chemical Communications, Journal Year: 2024, Volume and Issue: unknown

Published: Jan. 1, 2024

Tetraene-linked diketopyrrolopyrrole (DPP)-based CMPs were developed via Knoevenagel condensation. The CMP has been characterized with NIR absorption (∼1200 nm) and high electrical conductivity (0.2 S m −1 ).

Language: Английский

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