EnergyChem, Journal Year: 2023, Volume and Issue: 5(6), P. 100112 - 100112
Published: Nov. 1, 2023
Language: Английский
EnergyChem, Journal Year: 2023, Volume and Issue: 5(6), P. 100112 - 100112
Published: Nov. 1, 2023
Language: Английский
Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 62(26)
Published: April 25, 2023
Abstract Photocatalytic oxygen reduction reaction (ORR) offers a promising hydrogen peroxide (H 2 O ) synthetic strategy, especially the one‐step two‐electron (2e − ORR route holds great potential in achieving highly efficient and selectivity. However, 2e is rarely harvested underlying mechanism for regulating pathways remains greatly obscure. Here, by loading sulfone units into covalent organic frameworks (FS‐COFs), we present an photocatalyst H generation via from pure water air. Under visible light irradiation, FS‐COFs exert superb yield of 3904.2 μmol h −1 g , outperforming most reported metal‐free catalysts under similar conditions. Experimental theoretical investigation reveals that accelerate separation photoinduced electron‐hole (e ‐h + pairs, enhance protonation COFs, promote adsorption Yeager‐type, which jointly alters process two‐step to one, thereby with high
Language: Английский
Citations
186Nature Catalysis, Journal Year: 2024, Volume and Issue: 7(2), P. 195 - 206
Published: Feb. 13, 2024
Language: Английский
Citations
166Water Research, Journal Year: 2023, Volume and Issue: 230, P. 119562 - 119562
Published: Jan. 2, 2023
Language: Английский
Citations
100Applied Catalysis B Environment and Energy, Journal Year: 2023, Volume and Issue: 342, P. 123340 - 123340
Published: Sept. 26, 2023
Language: Английский
Citations
99Advanced Functional Materials, Journal Year: 2023, Volume and Issue: 34(12)
Published: Dec. 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.
Language: Английский
Citations
93Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(22)
Published: Feb. 28, 2024
Abstract The solar‐driven photocatalytic production of hydrogen peroxide (H 2 O ) from water and oxygen using semiconductor catalysts offers a promising approach for converting solar energy into storable chemical energy. However, the efficiency H is often restricted by low photo‐generated charge separation, slow surface reactions inadequate stability. Here, we developed mixed‐linker strategy to build donor‐acceptor‐acceptor (D–A–A) type covalent organic framework (COF) photocatalyst, FS‐OHOMe‐COF. FS‐OHOMe‐COF structure features extended π–π conjugation that improves mobility, while introduction sulfone units not only as active sites facilitates with but also bolsters stability through increased interlayer forces. resulting has exciton binding energy, long excited‐state lifetime high photo‐stability leads performance (up 1.0 mM h −1 an output 19 after 72 hours irradiation. Furthermore, catalyst demonstrates stability, which sustained activity over 192 experiment.
Language: Английский
Citations
62Nature Communications, Journal Year: 2024, Volume and Issue: 15(1)
Published: March 26, 2024
Hydrogen peroxide photosynthesis suffers from insufficient catalytic activity due to the high energy barrier of hydrogen extraction H2O. Herein, we report that mechanochemically synthesized keto-form anthraquinone covalent organic framework which is able directly synthesize H2O2 (4784 μmol h-1 g-1 at λ > 400 nm) oxygen and alkaline water (pH = 13) in absence any sacrificial reagents. The strong alkalinity resulted formation OH-(H2O)n clusters water, were adsorbed on keto moieties within then dissociated into O2 active hydrogen, because was largely lowered. produced reacted with generate anthrahydroquinone, subsequently oxidized by produce H2O2. This study ultimately sheds light importance H2O for demonstrates synthesis achievable under conditions.
Language: Английский
Citations
55Proceedings of the National Academy of Sciences, Journal Year: 2023, Volume and Issue: 120(6)
Published: Feb. 2, 2023
Photosynthesis of hydrogen peroxide (H2O2) by selective oxygen reduction is a green and cost-effective alternative to the energy-intensive anthraquinone process. Although inexpensive polymeric graphitic carbon nitride (g-C3N4) exhibits ability produce H2O2, its disordered amorphous structure leads high recombination rate photogenerated carriers hinders charge transfer between layers. Herein, we predict that stacked g-C3N4 with ion intercalation (K+ I-) can improve carrier separation multiscale computational simulations. The electronic structures were tailored modified intercalating K+ I- into layer-by-layer structures. Guided predictions, achieved efficient solar-driven H2O2 production employing this facile ion-intercalated crystalline g-C3N4. An 13.1 mM g-1 h-1 an apparent quantum yield 23.6% at 400 nm obtained. synergistic effects crystallinity regulation dual interstitial doping engineering triggered formation new light absorption centers, establishment rapid diffusion channels, enhancement two-electron characteristics. This work sheds on tuning broadens design principles organic-conjugated polymer photocatalysts for environmental remediation energy conservation.
Language: Английский
Citations
53Nature Communications, Journal Year: 2024, Volume and Issue: 15(1)
Published: June 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 .
Language: Английский
Citations
41Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(23)
Published: April 3, 2024
Bipyridine-based covalent organic frameworks (COFs) have emerged as promising contenders for the photocatalytic generation of hydrogen peroxide (H
Language: Английский
Citations
39