Decoupling Interlayer Interactions Boosts Charge Separation in Covalent Organic Frameworks for High‐Efficiency Photocatalytic CO2 Reduction DOI

Liyang Qin,

Dazhong Sun, D.L. Ma

et al.

Advanced Materials, Journal Year: 2025, Volume and Issue: unknown

Published: April 29, 2025

Abstract Covalent organic frameworks (COFs) have emerged as promising photocatalysts owing to their structural diversity, tunable bandgaps, and exceptional light‐harvesting capabilities. While previous studies primarily focus on developing narrow‐bandgap COFs for broad‐spectrum solar energy utilization, the critical role of interlayer coupling in regulating charge transfer dynamics remains unclear. Conventional monolayer‐based theoretical models inadequately address effects that potentially hindering intralayer electron transport catalytic active sites. This work employs density functional theory (DFT) calculations investigate influence interactions imine‐based COFs. Theoretical analyses reveal bilayer architectures exhibit pronounced interference intramolecular processes which has not been observed monolayer models. Based these mechanistic insights, this designs two isomeric pyrene‐based incorporating identical donor (pyrene) acceptor (nickel bipyridine) units but with distinct strengths. Strikingly, optimized COF weakened demonstrates photocatalytic CO 2 reduction performance, achieving a evolution rate 553.3 µmol g −1 h 94% selectivity under visible light irradiation without additional photosensitizers or co‐catalysts. These findings establish engineering crucial design principle high‐performance COF‐based conversion applications.

Language: Английский

Zwitterionic covalent organic framework triggering enhanced H2O2 photoproduction via controllable built-in electric field design DOI
Chao Yang,

Linxiao Hou,

Jiale Yang

et al.

Chemical Engineering Journal, Journal Year: 2025, Volume and Issue: unknown, P. 161631 - 161631

Published: March 1, 2025

Language: Английский

Citations

0
Photoresponsive Behavior of Triphenylamine‐Based Organic Small Molecule Emitters Involving a Photo‐Induced Charge‐Transfer Complexation Mechanism under UV Light DOI Open Access
Xiaoteng Jia, Yukun Yuan, Qi Lin

et al.

Chinese Journal of Chemistry, Journal Year: 2025, Volume and Issue: unknown

Published: March 20, 2025

Comprehensive Summary Stimuli‐responsive organic luminescent materials exhibit significant sensitivity to various external stimuli, among which their excellent photosensitivity is particularly prominent. This unique feature gives them great potential for applications. Herein, five small molecule emitters based on triphenylamine derivatives have been synthesized via Suzuki‐coupling reaction. These molecules fluorescence properties with quantum yields ( Φ ) all reaching over 90%. When irradiated a 365 nm UV lamp, interesting photochromic phenomena occurred in chloroform solutions. phenomenon has studied intensively by UV‐vis absorption and spectroscopy, EPR measurements, density functional theory calculations, finally, the group was used as photoinitiation precursor electron donor, photo‐induced charge transfer complex (PCTC) initiated donor successfully constructed.

Language: Английский

Citations

0
Coupling Ionic Polarization, Electron Sponge Effect by One‐Pot Hypercrosslinking, Pyridiniumnation of Photosensitizer‐Based Porous Organic Polymers for Enhancing Advanced Oxidation Process DOI

Wuzi Zhao,

Lixuan Kan,

Danfeng Wang

et al.

Advanced Functional Materials, Journal Year: 2025, Volume and Issue: unknown

Published: April 4, 2025

Abstract Porous organic polymers (POPs) are emerging as up‐and‐coming photocatalysts for energy conversion, and environmental treatment. However, attention to simultaneously improving photoinduced charge separation, transfer, interfacial reaction is markedly lagged. Herein, the strategy of coupling ionic polarization, electron sponge effect enhancing built‐in electric field (BIEF), surface mass transfer process POPs proposed, which can be realized by a one‐pot post‐pyridiniumnation, Friedel‐Craft reaction. This method endows polarization elevating BIEF boosting separation/migration. The pyridiniumnation not only induces allow shallow trap free electrons but also effectively reduces oxygen adsorption energy, pertinent intermediates, thus leading stronger in 2.73‐fold neutral polymer strengthened O 2 activation. Additionally, photothermal performance with up 15 °C increment contributes enhancement photocatalysis. Consequently, iBPyP‐33 exhibits an unprecedentedly efficient photodegradation 100 ppm bisphenol A (BPA) just 20 min, photosynthesis H rate 3070 µmol g −1 h air, 6583 aided sodium ethylenediaminetetraacetic acid. study provides fresh, valuable insights into design high efficiency.

Language: Английский

Citations

0
One-Step Precipitation and Coordination Mechanism for Highly Efficient Fe-Cu Separation in Acidic Wastewater DOI

Xiaoyun Liu,

Wenchao Zhang, Hongrui Xiang

et al.

Published: Jan. 1, 2025

Language: Английский

Citations

0
Decoupling Interlayer Interactions Boosts Charge Separation in Covalent Organic Frameworks for High‐Efficiency Photocatalytic CO2 Reduction DOI

Liyang Qin,

Dazhong Sun, D.L. Ma

et al.

Advanced Materials, Journal Year: 2025, Volume and Issue: unknown

Published: April 29, 2025

Abstract Covalent organic frameworks (COFs) have emerged as promising photocatalysts owing to their structural diversity, tunable bandgaps, and exceptional light‐harvesting capabilities. While previous studies primarily focus on developing narrow‐bandgap COFs for broad‐spectrum solar energy utilization, the critical role of interlayer coupling in regulating charge transfer dynamics remains unclear. Conventional monolayer‐based theoretical models inadequately address effects that potentially hindering intralayer electron transport catalytic active sites. This work employs density functional theory (DFT) calculations investigate influence interactions imine‐based COFs. Theoretical analyses reveal bilayer architectures exhibit pronounced interference intramolecular processes which has not been observed monolayer models. Based these mechanistic insights, this designs two isomeric pyrene‐based incorporating identical donor (pyrene) acceptor (nickel bipyridine) units but with distinct strengths. Strikingly, optimized COF weakened demonstrates photocatalytic CO 2 reduction performance, achieving a evolution rate 553.3 µmol g −1 h 94% selectivity under visible light irradiation without additional photosensitizers or co‐catalysts. These findings establish engineering crucial design principle high‐performance COF‐based conversion applications.

Language: Английский

Citations

0