Reprogram Local Electronic Configuration in Multicomponent Covalent–Organic Frameworks for Efficient Hydrogen Peroxide Photoproduction

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

Published: Feb. 19, 2025

Covalent organic frameworks (COFs) have recently demonstrated significant potential for photocatalysis. Optimizing the local electronic environment in COFs has been considered to be critical enhancing photocatalytic activity. Here, we report a one-pot "grafting-to" strategy reprogram configurations of series isoreticular multicomponent by introducing electron-donating or electron-withdrawing groups into pores transform photoinert photoactive and form intramolecular donor–acceptor (D-A) structures. Such D-A structures enhanced overall hydrogen peroxide photoproduction facilitating charge carrier separation optimizing band achieve oxygen reduction reaction water oxidation simultaneously. Notably, one incorporated with 2-aminothiazole exhibits production rate 3701 μmol g–1 h–1 solar-to-chemical conversion efficiency 0.13% without use any sacrificial reagents, it 100% bacterial killing rates remarkable >90% biofilm removal capability. This COF modification strategy, which not reported before, offers unique approach constructing highly active photocatalysts containing great future design antibacterial therapies.

Language: Английский

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Engineering the S-scheme heterojunction modulating the charge density of the central carbon atom of half-metallic carbon nitride for boosting CO2 photoreduction

Applied Catalysis B Environment and Energy, Journal Year: 2025, Volume and Issue: unknown, P. 125200 - 125200

Published: Feb. 1, 2025

Language: Английский

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Elucidating Unique Synergic Enhancement Effect for H₂O₂ Production in Crystalline Carbon Nitride with Cyanamide‐Defect and Heptazine‐Triazine Junction

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

Published: Feb. 28, 2025

Abstract Cyanamide‐defect and heptazine/triazine (H/T) junction in g‐C 3 N 4 (CN) have commonly been considered as an effective strategy for solar‐driven artificial H 2 O photosynthesis. However, their synergistic effect is still ambiguous regarding how to manipulate free electrons effectively participate the reduction . Herein, through alkali‐salt‐assist‐thermal polymerization approach, a series of samples with cyanamide‐defect, H/T aredeveloped. Subsequently, it demonstrated that appropriate ratio cyanamide defect crystalline CN can respectively facilitate formation at shorter longer lifetime scales due different strength driving forces. These synergically direct 2e − stepwise radical process efficient production. Eventually, elucidate optimal photocatalyst, owing its structure proper defect, achieved remarkable yield 60.03 mmol h −1 g quantum efficiency 43.7% 420 nm solar‐to‐chemical‐conversion 2.55% under AM 1.5G irradiation. This work will open bright avenue design organic photocatalysts charge carriers engaging surface reaction.

Language: Английский

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Impact of the Donor–Acceptor Structure on Photocatalytic Hydrogen Generation by Polyfluorene Polymer Dots

ACS Applied Polymer Materials, Journal Year: 2025, Volume and Issue: unknown

Published: March 4, 2025

Organic semiconductor polymers have garnered significant attention within the realm of photocatalytic hydrogen generation. Researchers designed numerous schemes to enhance efficiency generation by leveraging tunable properties their main chains. The donor–acceptor (D–A) strategy is a recognized approach for tuning photoelectric polymer semiconductors; however, its application organic demands thorough investigation. Here, we use polyfluorene derivatives study effect D–A structure on properties. After these were prepared into dots (Pdots) through nanoprecipitation method, they exhibited excellent We found that PFO-Pdots obtained rate 0.74 mmol g–1 h–1, and PFBT-Pdots with had about three times (2.23 h–1) PFO-Pdots, while PFVA-Pdots in presence D–D only one-half (0.34 PFO-Pdots. These results indicated plays critical role enhancing performance polymers. This will motivate take advantage structural tunability enable further development field

Language: Английский

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Visible-light-induced C2-selective trifluoromethylation of indoles catalyzed by copper-containing covalent organic frameworks

Journal of Catalysis, Journal Year: 2025, Volume and Issue: unknown, P. 116077 - 116077

Published: March 1, 2025

Language: Английский

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