Advances of MOFs and COFs for photocatalytic CO2 reduction, H2 evolution and organic redox transformations

Coordination Chemistry Reviews, Journal Year: 2023, Volume and Issue: 490, P. 215210 - 215210

Published: May 21, 2023

Language: Английский

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Linker Engineering for Reactive Oxygen Species Generation Efficiency in Ultra-Stable Nickel-Based Metal–Organic Frameworks

Journal of the American Chemical Society, Journal Year: 2023, Volume and Issue: 145(34), P. 18931 - 18938

Published: Aug. 17, 2023

Interfacial charge transfer on the surface of heterogeneous photocatalysts dictates efficiency reactive oxygen species (ROS) generation and therefore aerobic oxidation reactions. Reticular chemistry in metal-organic frameworks (MOFs) allows for rational design donor-acceptor pairs to optimize interfacial charge-transfer kinetics. Herein, we report a series isostructural fcu-topology Ni8-MOFs (termed JNU-212, JNU-213, JNU-214, JNU-215) with linearly bridged bipyrazoles as organic linkers. These crystalline can maintain their structural integrity 7 M NaOH at 100 °C 24 h. Experimental studies reveal that linker engineering by tuning electron-accepting capacity pyrazole-bridging units renders these significantly improved separation under visible-light irradiation. Among them, one containing benzoselenadiazole unit (JNU-214) exhibits best photocatalytic performance benzylamines conversion rate 99% Recycling experiments were carried out confirm stability reusability JNU-214 robust catalyst. Significantly, systematic modulation bridging donor-acceptor-donor MOFs provides new pathway develop viable noble-metal-free

Language: Английский

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Donor-acceptor-based conjugated polymers for photocatalytic energy conversion

EnergyChem, Journal Year: 2023, Volume and Issue: 6(1), P. 100116 - 100116

Published: Nov. 29, 2023

Language: Английский

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Relative Local Electron Density Tuning in Metal‐Covalent Organic Frameworks for Boosting CO₂ Photoreduction

Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 62(44)

Published: Sept. 15, 2023

The high local electron density and efficient charge carrier separation are two important factors to affect photocatalytic activity, especially for the CO2 photoreduction reaction. However, systematic studies on structure-functional relationship regarding above based precisely structure model rarely reported. Herein, as a proof-of-concept, we developed new strategy evaluation of by controlling relative electron-deficient (ED) electron-rich (ER) intensity monomer at molecular level three rational-designed vinylene-linked sp2 carbon-covalent organic frameworks (COFs). As expected, as-prepared carbon-conjugated metal-covalent framework (MCOFs) (VL-MCOF-1) with junction exhibited excellent activities -to-HCOOH conversion (283.41 μmol g-1 h-1 ) selectivity 97.1 %, much higher than VL-MCOF-2 g-C34 N6 -COF, which is due synergistic effect multi-electronic metal clusters (Cu3 (PyCA)3 (PyCA=pyrazolate-4-carboxaldehyde) strong ER roles cyanopyridine units ED active sites, well boosted photo-induced efficiency vinyl connection increased light utilization ability. These results not only provide regulating electron-density distribution photocatalysts but also offers profound insights clusters-based COFs effective conversion.

Language: Английский

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Introduction of electron-deficient unit in resorcinol-formaldehyde resin to construct donor–acceptor conjugated polymer for enhancing photocatalytic H₂O₂ production

Journal of Materials Chemistry A, Journal Year: 2024, Volume and Issue: 12(14), P. 8420 - 8428

Published: Jan. 1, 2024

Intramolecular donor–acceptor conjugated polymer was constructed in resorcinol-formaldehyde resin by embedding benzothiadiazole, which can reduce the Gibbs free energy for two-electron oxygen reduction and improve photocatalytic H 2 O evolution.

Language: Английский

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Semiconductor cooperative photocatalysis with TEMPO

Trends in Chemistry, Journal Year: 2024, Volume and Issue: 6(3), P. 115 - 127

Published: Feb. 20, 2024

Language: Английский

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Strategy to Efficient Photodynamic Therapy for Antibacterium: Donor‐Acceptor Structure in Hydrogen‐Bonded Organic Framework

Advanced Materials, Journal Year: 2024, Volume and Issue: 36(35)

Published: June 24, 2024

While the construction of a donor-acceptor (D-A) structure has gained great attention across various scientific disciplines, such structures are seldomly reported within field hydrogen-bonded organic frameworks (HOFs). Herein, D-A based HOF is synthesized, where adjacent pairs connected by hydrogen bonds instead conventionally employed covalent bonds. This structural feature imparts material with reduced energy gap between excited state and triplet state, thereby facilitating intersystem crossing (ISC) boosting generation rate single oxygen (quantum yield = 0.98). Consequently, resulting shows high performance for antimicrobial photodynamic therapy (PDT). The impact moiety evident when comparing this finding to parallel study conducted on an isoreticular without structure. presented here provides in-depth insights into photophysical properties pair in network, opening new avenue design innovative materials efficient PDT.

Language: Английский

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Facile synthesis of a nitrogen-rich covalent organic framework for the efficient capture of iodine

Journal of Materials Chemistry A, Journal Year: 2024, Volume and Issue: 12(17), P. 10539 - 10553

Published: Jan. 1, 2024

The effective containment and storage of iodine is important, fulfilling both the roles managing nuclear waste ensuring safe utilization radioactive isotopes in medicine.

Language: Английский

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Tuning the exciton binding energy of covalent organic frameworks for efficient photocatalysis

Chinese Chemical Letters, Journal Year: 2023, Volume and Issue: 35(2), P. 108356 - 108356

Published: March 22, 2023

Language: Английский

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De Novo Synthesis of Acridone-Based Zn-Metal–Organic Framework (Zn-MOF) as a Photocatalyst: Application for Visible Light-Mediated Oxidation of Sulfides and Enaminones

ACS Applied Materials & Interfaces, Journal Year: 2024, Volume and Issue: 16(3), P. 3348 - 3358

Published: Jan. 9, 2024

Acridone, a cyclic analogue of benzophenone that undergoes efficient intersystem crossing (ISC) to the triplet-excited state with near-unity quantum yield, was elaborated as 3-connecting triacid linker, i.e., H3AcTA, develop photocatalytic metal–organic framework (MOF) for energy transfer applications; linker inherently features concave shapes, an attribute is important construction MOFs significant porosity. Metal ion (Zn2+)-assisted self-assembly yielded Zn-MOF, Zn-AcTA, solvent-accessible volume ca. 31%. The protection acridone chromophore in MOF conjunction wider cross-section its absorption visible region renders excellent heterogeneous photosensitizer singlet oxygen (1O2) generation by ground-state triplet (3O2). It shown Zn-MOF can be applied photosensitizing catalyst light-mediated oxidation various sulfides sulfoxides and enaminones amino-esters via 1,2-acyl migration. further demonstrated photocatalyst easily recycled without any loss catalytic activity structural integrity. Based on mechanistic investigations, 1O2 established reactive species reactions. results constitute first demonstration rational development based oxidations mediated 1O2.

Language: Английский

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