Advanced Materials, Journal Year: 2024, Volume and Issue: unknown
Published: Nov. 7, 2024
Covalent organic frameworks (COFs) offer a compelling platform for the efficient photosynthesis of hydrogen peroxide (H
Language: Английский
Advanced Materials, Journal Year: 2024, Volume and Issue: unknown
Published: Nov. 7, 2024
Covalent organic frameworks (COFs) offer a compelling platform for the efficient photosynthesis of hydrogen peroxide (H
Language: Английский
Advanced Energy Materials, Journal Year: 2024, Volume and Issue: 14(23)
Published: April 3, 2024
Abstract Solar energy can be utilized in photocatalysis technology to realize light‐driven hydrogen peroxide (H 2 O ) production, a green chemical synthesis route. Designing high‐performance photocatalysts is critical achieving practical solar H production. During the past decade, significant research progress made photocatalytic materials for Particularly 2D materials‐based stand out due their unique physical and properties. This review highlights intricate relationship between material innovation photochemical It starts with fundamental principles of generation, focusing on crucial steps such as photon absorption, carrier dynamics, surface reactions, challenges that solve at each step. Then, various production are introduced detail. Engineering strategies optimize performance discussed afterward. Finally, future opportunities designing outlined. expected inspire engineering conversion other chemicals.
Language: Английский
Citations
81ACS Catalysis, Journal Year: 2024, Volume and Issue: 14(7), P. 4728 - 4737
Published: March 13, 2024
Imine-linked isomeric covalent organic frameworks (COFs) with opposite linkage orientations are not rare, but their structure and photocatalytic property corrections still puzzling, let alone the emerging photosynthetic H2O2 performance. Herein, a pair of COFs (TB-COF TA-COF) reversed imine linkages was fabricated. Compared to TA-COF, TB-COF exhibited larger dipole moments better charge carrier separation efficiency, resulting in superior photosynthesis capability via dominant oxygen reduction reaction (ORR) paths (O2–O2•––H2O2 O2–O2•––O21–H2O2) feeble water oxidation (WOR) paths. With no sacrificial agents air, rates were 5186 μmol g–1 h–1 4111 natural seawater, respectively. The seawater-produced can be directly utilized for tetracycline degradation, manifesting big picture wastewater treatment by H2O2. Theoretical calculations revealed that hydroxyl-rich benzene ring photooxidation part triazine unit primary photoreduction part. Through linkage-orientation regulation, electronic structures, migration property, energy barrier rate determination step 2e– ORR WOR well-modulated. current work provides insight into effect orientation on performance may enlighten design catalysts photosynthesis.
Language: Английский
Citations
38Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(32)
Published: May 13, 2024
Abstract Covalent organic frameworks (COFs) are promising photocatalysts for H 2 O production from water via oxygen reduction reaction (ORR). The design of COFs efficient indubitably hinges on an in‐depth understanding their ORR mechanisms. In this work, taking imine‐linked COF as example, we demonstrate that protonation the functional units such imine, amine, and triazine, is a highly strategy to upgrade activity levels synthesis. not only extends light absorption but also provides proton sources directly participate in generation. Notably, simplifies pathways , i.e. indirect superoxide radical ( ) mediated route direct one‐step two‐electron route. Theoretical calculations confirm favors synthesis due easy access protons near sites removes energy barrier generating *OOH intermediate. These findings extend mechanistic insight into photosynthesis provide rational guideline upgradation COFs.
Language: Английский
Citations
35Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(24)
Published: April 12, 2024
Photocatalytic oxygen reduction reactions and water oxidation are extremely promising green approaches for massive H
Language: Английский
Citations
34Applied Catalysis B Environment and Energy, Journal Year: 2024, Volume and Issue: 358, P. 124366 - 124366
Published: July 3, 2024
Language: Английский
Citations
33Advanced Energy Materials, Journal Year: 2024, Volume and Issue: 14(40)
Published: July 18, 2024
Abstract The integration of electron donor (D) and acceptor (A) units into covalent organic frameworks (COFs) has received increasing interest due to its potential for efficient photocatalytic hydrogen (H 2 ) evolution from water. Nevertheless, the advancement D–A COFs is still constrained by limited investigations on engineering, which enables highly effective charge transfer pathways in deliver photoexcited electrons a preferential orientation enhance performance. Herein, two systems with D–A–A configurations based molecular engineering strategy are proposed construct three distinct COFs. Specifically, TAPPy‐DBTDP‐COF merging one pyrene‐based benzothiadiazole acceptors realized an average H rate 12.7 mmol h −1 g under visible light, among highest ever reported typical D–A‐type COF systems. combination experimental theoretical analysis signifies crucial role dual‐acceptor arrangement promoting exciton dissociation carrier migration. These findings underscore significant structural design, conducive separation holes resulting superior activities.
Language: Английский
Citations
33Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: unknown
Published: Aug. 20, 2024
Photocatalytic synthesis of H
Language: Английский
Citations
22Advanced Functional Materials, Journal Year: 2024, Volume and Issue: 34(29)
Published: March 14, 2024
Abstract Porous organic polymers have an outstanding performance in the field of photocatalysis with advantage diverse structure composition and purposeful molecular design. However, inherent high impedance poor electrical conductivity semiconductors still restrict charge transfer efficiency thus discount photocatalytic performance. Herein, study reports a highly conductive covalent triazine framework (CTF) loading carbon quantum dots (CQDs) into porous as electron transport medium. The addition CQDs (0.5 wt%) can enhance electronic CTF by tenfold. In addition, as‐prepared CQD‐CTFs express much‐promoted separation efficiency. Furthermore, embedded improve oxidization capacity increase affinity H + due to more negative zeta potential. enhanced oxidizing ability increased are positive for water oxidation reaction (WOR) oxygen reduction (ORR) process hydrogen peroxide (H 2 O ) generation, respectively. optimized CQD‐CTF exhibits generation rate up 1036 µmol g −1 h pure without any sacrificial agent under visible light, which is 4.6 times than pristine CTF. This work provides new idea efficient production semiconductors.
Language: Английский
Citations
21Journal of the American Chemical Society, Journal Year: 2024, Volume and Issue: unknown
Published: April 11, 2024
Hydrogen peroxide (H
Language: Английский
Citations
21Applied Catalysis B Environment and Energy, Journal Year: 2024, Volume and Issue: 355, P. 124077 - 124077
Published: May 14, 2024
Language: Английский
Citations
21