Metal-free Fenton-like photocatalysts based on covalent organic frameworks

Liao, Qiaobo; Wang, Dongni; Ke, Can; Zhang, Yiying; Han, Qinwen; Zhang, Yifan; Xi, Kai

doi:10.1016/j.apcatb.2021.120548

Cited by 48 publications

(22 citation statements)

References 69 publications

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“…To elucidate the photodegradation mechanism in depth, we further investigated the main active species during the photodegradation of RhB over COF-HFeTBD in the presence of H 2 O 2 under visible light irradiation via electron paramagnetic resonance spectroscopy (EPR) measurements. 5,5-Dimethyl-1-pyrroline-N-oxide (DMPO) was selected as the spin-trapping adduct to detect ·O 2 – in methanol solutions and ·OH in aqueous solutions, respectively, and 2,2,6,6-tetramethylpiperidine (TEMP) was used to capture 1 O 2 in aqueous solutions . In the presence of the COF-HFeTBD/H 2 O 2 catalytic system, a quartet EPR signal in a 1:2:2:1 ratio characteristic for ·OH adducts can be observed after visible light irradiation (Figure a).…”

Section: Resultsmentioning

confidence: 99%

“…It can be found that the average fluorescence lifetimes increased significantly with the incorporation of metal ions in the porphyrin core, indicating that the − in methanol solutions and •OH in aqueous solutions, respectively, and 2,2,6,6-tetramethylpiperidine (TEMP) was used to capture 1 O 2 in aqueous solutions. 33 In the presence of the COF-HFeTBD/H 2 O 2 catalytic system, a quartet EPR signal in a 1:2:2:1 ratio characteristic for •OH adducts can be observed after visible light irradiation (Figure 6a). Interestingly, no apparent •OH signals were observed in the dark, suggesting that •OH reactive radicals could be generated in the presence of visible light irradiation.…”

Section: Optical and Electrochemical Featuresmentioning

confidence: 99%

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Crystalline Covalent Organic Frameworks Based on Mixed Metallo- and Tetrahydroporphyrin Monomers for Use as Efficient Photocatalysts in Dye Pollutant Removal

Liu

Chen

et al. 2022

Crystal Growth & Design

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Unique features, including a high specific surface area, great stability, and crystallinity, make covalent organic frameworks (COFs) intriguing sorbents and catalysts in light-driven water pollutant degradation. Inspired by the light absorption capability of porphyrin derivatives and the carrier separation ability of a donor−acceptor (D−A) configuration, we constructed two-dimensional porphyrin donor-based D−A COFs: COF-HTBD involving only tetrahydroporphyrins and COF-HMTBD (M = Co, Fe, Cu) involving both tetrahydro-and metalloporphyrins via a mixed porphyrin monomer strategy. The monomer 2,1,3-benzothiadiazole-4,7dicarboxaldehyde (BD) is incorporated as an electron accepting moiety. Interestingly, COF-HTBD, COF-HCuTBD, and COF-HFeTBD exhibit staggered stacking, while the stacking model of COF-HCoTBD transforms from staggered to eclipsed. Notably, COF-HFeTBD demonstrates excellent activities and stabilities toward visible light-driven photocatalytic rhodamine B (RhB) degradation in aqueous solutions with H 2 O 2 present (100% removal in 3 h). Overall, this work provides an interesting strategy for the construction of D−A-type porphyrin COFs for dye pollutant removal.

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Section: Resultsmentioning

confidence: 99%

Section: Optical and Electrochemical Featuresmentioning

confidence: 99%

Crystalline Covalent Organic Frameworks Based on Mixed Metallo- and Tetrahydroporphyrin Monomers for Use as Efficient Photocatalysts in Dye Pollutant Removal

Liu

Chen

et al. 2022

Crystal Growth & Design

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“…The Fenton-like photocatalytic process is one of the advanced techniques that exhibits unique advantages of strong oxidation capacity, high reaction rate, and mild reaction conditions. [121][122][123][124] Based on this view, Zhang et al reported a highly active Fenton-like hybrid photocatalyst of NH 2 -MIL88B@TpPa-1-COF, which was constructed according to the process in Figure 7a. [125] The photocatalytic performance of as-synthesized hybrid materials was evaluated by the photocatalytic degradation of tetracycline (TC).…”

Section: Photocatalytic Degradationmentioning

confidence: 99%

Progress in Hybridization of Covalent Organic Frameworks and Metal–Organic Frameworks

Deng

Wang

Xiao

et al. 2022

Small

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Metal–organic frameworks (MOFs) and covalent organic frameworks (COFs) hybrid materials are a class of porous crystalline materials that integrate MOFs and COFs with hierarchical pore structures. As an emerging porous frame material platform, MOF/COF hybrid materials have attracted tremendous attention, and the field is advancing rapidly and extending into more diverse fields. Extensive studies have shown that a broad variety of MOF/COF hybrid materials with different structures and specific properties can be synthesized from diverse building blocks via different chemical reactions, driving the rapid growth of the field. The allowed complementary utilization of π‐conjugated skeletons and nanopores for functional exploration has endowed these hybrid materials with great potential in challenging energy and environmental issues. It is necessary to prepare a “family tree” to accurately trace the developments in the study of MOF/COF hybrid materials. This review comprehensively summarizes the latest achievements and advancements in the design and synthesis of MOF/COF hybrid materials, including COFs covalently bonded to the surface functional groups of MOFs (MOF@COF), MOFs grown on the surface of COFs (COF@MOF), bridge reaction between COF and MOF (MOF+COF), and their various applications in catalysis, energy storage, pollutant adsorption, gas separation, chemical sensing, and biomedicine. It concludes with remarks concerning the trend from the structural design to functional exploration and potential applications of MOF/COF hybrid materials.

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“…Unlike the metal-based approaches, metal free system operates in broad range of pH scale and avoids the risk of metal leaching. 2 Additionally, heterogeneous metal-free catalysts are easily isolated from the reaction mixtures and readily employed for numerous cycles, saving energy, time, and labor while preparing the photocatalysis in contrast to homogenous. Only a limited photocatalyst are reported for Fenton-like reactions that produce reactive radicals under visible light.…”

Section: Introductionmentioning

confidence: 99%

Mechanically Activated Covalent Organic Framework as Metal Free Photocatalyst for Continuous Flow Fenton-like Degradation of Organic Pollutants and Hexavalent Chromium Reduction

Gogoi

Jena

Singh

et al. 2023

Preprint

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A highly active photocatalyst is unveiled for the Fenton-like reactions in visible light. A metal-free covalent organic framework (COF) was highly active via a novel mechanical pulverization process. Under visible light, the activity of pulverized COF reached an apparent quantum yield of 41% for Fenton-like degradation. The exceptional performance is due to the conduction band's induced high excited electron density. The outstanding performance does not require pH adjustment by external means, unlike metal-based photocatalysts. The pulverized COF can be recycled up to five times. For industrial scale implementation, the photocatalyst outperformed in a continuous flow channel. The photocatalytic space-time yield (PSTY) was increased by 28 times over conventional batch photocatalysis. For successful chemical reactions, an exceedingly small amount of photocatalyst is required. Additionally, a very high photoreduction rate was also observed for hexavalent chromium, which was significantly better than the parent COF.

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Metal-free Fenton-like photocatalysts based on covalent organic frameworks

Cited by 48 publications

References 69 publications

Crystalline Covalent Organic Frameworks Based on Mixed Metallo- and Tetrahydroporphyrin Monomers for Use as Efficient Photocatalysts in Dye Pollutant Removal

Crystalline Covalent Organic Frameworks Based on Mixed Metallo- and Tetrahydroporphyrin Monomers for Use as Efficient Photocatalysts in Dye Pollutant Removal

Progress in Hybridization of Covalent Organic Frameworks and Metal–Organic Frameworks

Mechanically Activated Covalent Organic Framework as Metal Free Photocatalyst for Continuous Flow Fenton-like Degradation of Organic Pollutants and Hexavalent Chromium Reduction

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