Boosting Exciton Dissociation and Charge Transfer in Fluorine-Substituted Covalent Organic Frameworks with Biomimetic Electron Pumps for Remarkable Photocatalytic Extraction of Uranium DOI

Gui-Hong Wu,

Fengtao Yu, Yiping Liu

et al.

ACS Applied Materials & Interfaces, Journal Year: 2024, Volume and Issue: 17(2), P. 3503 - 3513

Published: Dec. 30, 2024

Visible-light-driven photocatalytic uranium extraction based covalent organic frameworks (COFs) are green and sustainable, but their performance is severely restricted by a strong exciton effect. Herein, inspired the physiology of cardiac pacing, novel fluorine-based COF (PyF-DaS-COF) with biomimetic electronic pump has been fabricated used for uranium. Both experimental theoretical calculations confirm that strongly electronegative fluorine plays crucial role in dissociation charge transfer. The enhanced electron push–pull effect increases intrinsic separation driving force separation. Furthermore, substitution thermodynamically favors generation *OOH intermediate reduction reaction. As result, PyF-DaS-COF achieves record k value (T = 293 K) 0.082 min–1 an capacity 991.5 mg g–1. Importantly, removal rate over 99% real uranium-containing wastewater. current work provides unique insights into designing effective COFs controlling radioactive contamination.

Language: Английский

Engineering exciton dissociation and intermolecular charge transfer to boost superoxide radical in conjugated microporous polymers for simultaneous elimination of coexisting contaminants DOI
Weijie Zhang,

Xinye Luo,

Luting Liu

et al.

Chemical Engineering Journal, Journal Year: 2024, Volume and Issue: 499, P. 156552 - 156552

Published: Oct. 11, 2024

Language: Английский

Citations

7
Facilitating Charge Separation of Donor–Acceptor Conjugated Microporous Polymers via Position Isomerism Strategy for Efficient CO2 Photoconversion DOI Open Access

Dandan Wang,

Xiaofei Yan,

Xinsheng Zhu

et al.

Catalysts, Journal Year: 2024, Volume and Issue: 14(10), P. 659 - 659

Published: Sept. 24, 2024

Photoreduction of CO2 into the chemical feedstocks fuels provides a green way to help solve both energy crisis and carbon emission issues. Nevertheless, undesirable charge separation migration, as well rapid reverse recombination results in unsatisfactory photocatalytic activity most conjugated microporous polymers (CMPs). Herein, pair donor–acceptor (D-A) CMPs for photoconversion was developed through position isomerism by altering linkage sites. The show that Py-D27F with 2,7-site exhibits completely structure large molecular dipole moment, thus significantly accelerating transfer. As result, achieves higher yield 320.9 μmol g−1 h−1 CO2-to-CO photoreduction (without addition any photosensitizers precious metals), which is about three-fold greater than Py-D36F (3,6-site linkage). This study valuable idea exploring outstanding CMP photocatalysts efficient processing photocatalysis.

Language: Английский

Citations

0
Prolonging triplet-state lifetimes to boost the energy and electron transfer in conjugated organic polymers for photocatalytic amide formation DOI
Weijie Zhang, Bingxin Wang, Luting Liu

et al.

Journal of Catalysis, Journal Year: 2024, Volume and Issue: unknown, P. 115898 - 115898

Published: Dec. 1, 2024

Language: Английский

Citations

0
Structural Regulation of Sulfone-Decorated Conjugated Polymers for Boosting Photocatalysis DOI
Weijie Zhang,

Xinye Luo,

Huijing Tang

et al.

Journal of Materials Chemistry A, Journal Year: 2024, Volume and Issue: unknown

Published: Dec. 17, 2024

The multifarious aromatic sulfone-decorated conjugated polymers (CPs) have recently been developed to enable them be employed in artificial photocatalysis with encouraging achievements.

Language: Английский

Citations

0
Boosting Exciton Dissociation and Charge Transfer in Fluorine-Substituted Covalent Organic Frameworks with Biomimetic Electron Pumps for Remarkable Photocatalytic Extraction of Uranium DOI

Gui-Hong Wu,

Fengtao Yu, Yiping Liu

et al.

ACS Applied Materials & Interfaces, Journal Year: 2024, Volume and Issue: 17(2), P. 3503 - 3513

Published: Dec. 30, 2024

Visible-light-driven photocatalytic uranium extraction based covalent organic frameworks (COFs) are green and sustainable, but their performance is severely restricted by a strong exciton effect. Herein, inspired the physiology of cardiac pacing, novel fluorine-based COF (PyF-DaS-COF) with biomimetic electronic pump has been fabricated used for uranium. Both experimental theoretical calculations confirm that strongly electronegative fluorine plays crucial role in dissociation charge transfer. The enhanced electron push–pull effect increases intrinsic separation driving force separation. Furthermore, substitution thermodynamically favors generation *OOH intermediate reduction reaction. As result, PyF-DaS-COF achieves record k value (T = 293 K) 0.082 min–1 an capacity 991.5 mg g–1. Importantly, removal rate over 99% real uranium-containing wastewater. current work provides unique insights into designing effective COFs controlling radioactive contamination.

Language: Английский

Citations

0