Killing two birds with one stone: State-of-the-art progress in dual-functional photoredox catalysis for solar fuel conversion and selective organic transformation DOI
Feng Niu, Wenguang Tu, Yong Zhou

et al.

EnergyChem, Journal Year: 2023, Volume and Issue: 5(6), P. 100112 - 100112

Published: Nov. 1, 2023

Language: Английский

Sulfone‐Modified Covalent Organic Frameworks Enabling Efficient Photocatalytic Hydrogen Peroxide Generation via One‐Step Two‐Electron O2 Reduction DOI
Yu Luo, Beiping Zhang, Chenchen Liu

et al.

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

186
Linkage-engineered donor–acceptor covalent organic frameworks for optimal photosynthesis of hydrogen peroxide from water and air DOI
Ruoyang Liu, Yongzhi Chen, Hongde Yu

et al.

Nature Catalysis, Journal Year: 2024, Volume and Issue: 7(2), P. 195 - 206

Published: Feb. 13, 2024

Language: Английский

Citations

166
Enhanced H2O2 utilization efficiency in Fenton-like system for degradation of emerging contaminants: Oxygen vacancy-mediated activation of O2 DOI
Xixi Chen, Wanyi Fu, Zhichao Yang

et al.

Water Research, Journal Year: 2023, Volume and Issue: 230, P. 119562 - 119562

Published: Jan. 2, 2023

Language: Английский

Citations

100
Highly crystalline carbon nitrogen polymer with a strong built-in electric fields for ultra-high photocatalytic H2O2 production DOI

Liang Jian,

Yuming Dong, Hui Zhao

et al.

Applied Catalysis B Environment and Energy, Journal Year: 2023, Volume and Issue: 342, P. 123340 - 123340

Published: Sept. 26, 2023

Language: Английский

Citations

99
Covalent Organic Frameworks Enable Sustainable Solar to Hydrogen Peroxide DOI
Deming Tan, Rong Zhuang, Ruichong Chen

et al.

Advanced 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

93
Mixed‐Linker Strategy for the Construction of Sulfone‐Containing D–A–A Covalent Organic Frameworks for Efficient Photocatalytic Hydrogen Peroxide Production DOI
C. Shu,

Xiaoju Yang,

Lunjie Liu

et al.

Angewandte 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

62
Keto-anthraquinone covalent organic framework for H2O2 photosynthesis with oxygen and alkaline water DOI Creative Commons

Xiangcheng Zhang,

Silian Cheng,

Chao Chen

et al.

Nature 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

55
Synergy of crystallinity modulation and intercalation engineering in carbon nitride for boosted H 2 O 2 photosynthesis DOI Creative Commons
Lianlian Liu, Fei Chen, Jing‐Hang Wu

et al.

Proceedings 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

53
A photocatalytic redox cycle over a polyimide catalyst drives efficient solar-to-H2O2 conversion DOI Creative Commons

Wenwen Chi,

Yuming Dong, Bing Liu

et al.

Nature 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

41
Pyridine‐Based Covalent Organic Frameworks with Pyridyl‐Imine Structures for Boosting Photocatalytic H2O2 Production via One‐Step 2e− Oxygen Reduction DOI
Weijian Wu, Zixuan Li, Shiyin Liu

et al.

Angewandte 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