Coordination Chemistry Reviews, Год журнала: 2024, Номер 506, С. 215694 - 215694
Опубликована: Фев. 14, 2024
Язык: Английский
Advanced Functional Materials, Год журнала: 2023, Номер 34(12)
Опубликована: Дек. 6, 2023
Abstract As a chemical product with rapidly expanding demand in the field of modern energy and environmental applications, hydrogen peroxide (H 2 O ) has garnered widespread attention. However, existing industrial production H is plagued by high consumption, harmful waste emission, severe safety issues, making it difficult to satisfy environmental/economic concept. Artificial photosynthesis offers viable strategy for green sustainable since uses sunlight as an source initiate reaction oxygen water produce . Among various photocatalysts, covalent organic frameworks (COFs), featuring highly ordered skeletons well‐defined active sites, have emerged promising photocatalysts production. This review presents nascent burgeoning area photocatalytic based on COFs. First, brief overview technology provided, followed detailed introduction principles evaluation generation. Subsequently, latest research progress judicious design COFs expounded, particular emphasis manipulating electronic structures redox sites. Finally, outlook challenges future opportunities proposed, hope stimulating further explorations novel molecular‐designed photosynthesis.
Язык: Английский
Процитировано
85
Advanced Energy Materials, Год журнала: 2024, Номер 14(23)
Опубликована: Апрель 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.
Язык: Английский
Процитировано
66
Advanced Functional Materials, Год журнала: 2024, Номер unknown
Опубликована: Март 10, 2024
Abstract Covalent organic frameworks (COFs) attract significant attention due to their ordered, crystalline, porous, metal‐free, and predictable structures. These unique characteristics offer great opportunities for the diffusion transmission of photogenerated charges during photocatalysis. Currently, a considerable number COFs are used as metal‐free semiconductor photocatalysts. This review aims understand relationships between structure photocatalysis performance provides in‐depth insight into synthetic strategy improve performance. Subsequently, focuses on structural motif in sustainable photocatalytic hydrogen evolution, carbon dioxide reduction, peroxide generation, compound transformations. Last, conjunction with progress achieved challenges yet be overcome, candid discussion is undertaken regarding field COF photocatalysis, accompanied by presentation potential research avenues future directions. seeks provide readers comprehensive understanding pivotal role robust guidance innovative utilization
Язык: Английский
Процитировано
61
Advanced Fiber Materials, Год журнала: 2024, Номер 6(2), С. 387 - 400
Опубликована: Янв. 9, 2024
Язык: Английский
Процитировано
54
Angewandte Chemie International Edition, Год журнала: 2024, Номер 63(19)
Опубликована: Март 16, 2024
Abstract Photocatalytic oxygen reduction to produce hydrogen peroxide (H 2 O ) is a promising route providing oxidants for various industrial applications. However, the lack of well‐designed photocatalysts efficient overall H production in pure water has impeded ongoing research and practical thrusts. Here we present cyanide‐based covalent organic framework (TBTN‐COFs) combining 2,4,6‐trimethylbenzene‐1,3,5‐tricarbonitrile (TBTN) benzotrithiophene‐2,5,8‐tricarbaldehyde (BTT) building blocks with water‐affinity charge‐separation. The ultrafast intramolecular electron transfer (<500 fs) prolonged excited state lifetime (748 ps) can be realized by TBTN‐COF, resulting hole accumulated BTT electron‐rich TBTN block. Under one sun, 11013 μmol h −1 g yield rate achieved without any sacrificial agent, outperforming most previous reports. Furthermore, DFT calculation situ DRIFTS spectrums suggesting Yeager‐type absorption *O ⋅ − intermediate cyanide active site, which prohibits formation superoxide radical revealing favored pathway.
Язык: Английский
Процитировано
41
Angewandte Chemie International Edition, Год журнала: 2024, Номер 63(15)
Опубликована: Фев. 15, 2024
Abstract Photocatalytic oxygen reductive H 2 O production is a promising approach to alternative industrial anthraquinone processes while suffering from the requirement of pure feedstock for practical application. Herein, we report spaced double hydrogen bond (IC−H‐bond) through multi‐component Radziszewski reaction in an imidazole poly‐ionic‐liquid composite (SI‐PIL‐TiO ) and levofloxacin hydrochloride (LEV) electron donor highly efficient selective photocatalytic air production. It found that IC−H‐bond formed by imino (−NH−) group SI‐PIL‐TiO carbonyl (−C=O) LEV can switch active sites characteristic covered state fully exposed one shield strong adsorption N air, propel intenser positive potential more orbitals binding patterns surface establish competitive selectivity chemisorption. Moreover, high enrichment as site 2e − reduction ensures rapid . Therefore, enables total utilization conversion efficiency 94.8 % direct reduction, achieving rate 1518 μmol/g/h 16 23 times compared without groups (PIL‐TiO TiO , respectively.
Язык: Английский
Процитировано
39
Angewandte Chemie International Edition, Год журнала: 2024, Номер 63(18)
Опубликована: Март 7, 2024
Constructing stable and efficient photocatalysts for H
Язык: Английский
Процитировано
35
ACS Catalysis, Год журнала: 2024, Номер 14(7), С. 4728 - 4737
Опубликована: Март 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.
Язык: Английский
Процитировано
35
Nature Communications, Год журнала: 2024, Номер 15(1)
Опубликована: Июнь 22, 2024
Abstract Circumventing the conventional two-electron oxygen reduction pathway remains a great problem in enhancing efficiency of H 2 O photosynthesis. A promising approach to achieve outstanding photocatalytic activity involves utilization redox intermediates. Here, we engineer polyimide aerogel photocatalyst with photoreductive carbonyl groups for non-sacrificial production. Under photoexcitation, on surface are reduced, forming an anion radical intermediate. The produced intermediate is oxidized by produce and subsequently restores group. high catalytic ascribed cycle mediated anion, which not only promotes adsorption but also lowers energy barrier reaction generation. An apparent quantum yield 14.28% at 420 ± 10 nm solar-to-chemical conversion 0.92% achieved. Moreover, demonstrate that mere 0.5 m self-supported exposed natural sunlight 6 h yields significant production 34.3 mmol −2 .
Язык: Английский
Процитировано
34
ACS Catalysis, Год журнала: 2024, Номер 14(10), С. 7736 - 7745
Опубликована: Май 2, 2024
Covalent organic frameworks (COFs) have emerged as promising candidates for solar-driven photosynthesis of hydrogen peroxide (H2O2), yet the development high-performance COFs tailored practical applications presents substantial challenges. This research introduces integration redox-active catechol moiety into a series (TPE-COF-OH, TPB-COF-OH, and TPP-COF-OH), serving pivotal active site photocatalytic oxygen (O2) reduction to H2O2 through reversible catechol-quinone interconversion mechanism. process facilitates transformation o-benzoquinone in presence molecular O2, while photoexcited electrons are utilized revert catechol, reducing energy barrier synthesis. Notably, TPB-COF-OH demonstrates an unparalleled production rate 6608 μmol h–1 g–1, outperforming its counterpart, TPB-COF-OMe, which lacks unit. Furthermore, achieves solar-to-chemical conversion efficiency 0.84%, marking highest value among COF-based photocatalysts production. investigation not only underscores critical role engineering enhancing COF performance but also broadens horizon technologies.
Язык: Английский
Процитировано
33