Porphyrin-Based Two-Dimensional Layered Metal–Organic Framework with Sono-/Photocatalytic Activity for Water Decontamination

Zhu, Zhong‐Hong; Liu, Yubo; Song, Changhui; Hu, Yating; Feng, Guangxue; Tang, Ben Zhong

doi:10.1021/acsnano.1c09301

Cited by 100 publications

(68 citation statements)

References 79 publications

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“…Diminished generation abilities were also observed in the same experiments using HHTP and TFPN (Figure S12). Therefore, the exceptional 1 O 2 generation ability originates from the novel crystalline framework of COF-316 m , coupled with US, which is comparable to porphyrin-based MOF and COF sonosensitizers. , To verify the structural maintenance of COF-316 m after US irradiation, PXRD and IR data were collected (Figure S13). There were no significant differences between before and after US irradiation.…”

Section: Resultsmentioning

confidence: 99%

Promoted Type I and II ROS Generation by a Covalent Organic Framework through Sonosensitization and PMS Activation

et al. 2022

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Reactive oxygen species (ROS) are one of the most useful chemicals in photo-therapeutic and catalytic applications. In order to effectively generate ROS, the role of light-absorbing photosensitizers or activators for pre-ROS sources like peroxymonosulfate (PMS) is significantly essential. Although metal-based ROS-generating materials have been widely utilized due to the affordable heavy atom effect or viable catalytic sites, the potential toxicity of leached metal ions can be sometimes an undesirable hazard to humans and ecosystems. Herein, we prepare a covalent organic framework (COF) that generates both type I and II ROS upon ultrasound irradiation. In addition, the COF effectively generated ROS through PMS activation even without light sources or catalytic metal sites. We also observed synergistic ROS generation by sonosensitization and PMS activation by the COF. This work is a demonstration of the COF material functioning as both a sonosensitizer and a PMS activator.

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Section: Resultsmentioning

confidence: 99%

Promoted Type I and II ROS Generation by a Covalent Organic Framework through Sonosensitization and PMS Activation

et al. 2022

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“…The peak at −80 ppm is designated for the silicon atom with unreacted −CH CH 2 , indicating that about 80% of vinyl groups are involved in the reaction based on the integration ratio in the solid-state 29 Si NMR spectrum. 53 The solid-state 13 C spectra of PCS-CZ-DCM and OVS are shown in Figure S2. The overlapping signal of 109.6−157.9 ppm from PCS-CZ-DCM can be considered to be the result of the aromatic rings from CZ-DCM and the sp 2 carbon atoms of the unreacted vinyl groups.…”

Section: T H Imentioning

confidence: 99%

“…1 H NMR (400 MHz, (CD 3 ) 2 SO), δ (ppm): 8.28 (d, J = 8 Hz, 4H), 8.10 (d, J = 16Hz, 2H), 7.75 (d, J = 4 Hz, 2H), 7.67 (d, J = 8 Hz, 2H), 7.52−7.56 (m, 6H), 7.38 (t, J = 16 Hz, 4H), 7.22 (d, J = 16 Hz, 2H), 6.99 (s, 2H). 13 Fabrication of PCS-CZ-DCM. PCS-CZ-DCM was synthesized from OVS and CZ-DCM by the Friedel−Crafts reaction.…”

Section: T H Imentioning

confidence: 99%

Organic–Inorganic Hybrid Near-Infrared Emitting Porous Polymer for Detection and Photodegradation of Antibiotics

Wang

Unno

Liu

2022

ACS Sustainable Chem. Eng.

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In this study, an organic semiconductor molecule of 2-(2,6-bis((E)-2-(5-(9H-carbazol-9-yl)thiophen-2-yl)vinyl)-4H-pyran-4ylidene)malononitrile (CZ-DCM) with hyperconjugated "D-π-A-π-D" electron distribution, near-infrared emission, and a large Stokes shift of 190 nm was successfully prepared by the Knoevenagel reaction of 2-(2,6-dimethyl-4H-pyran-4-ylidene)malononitrile with 5-(9H-carbazol-9yl)thiophene-2-carbaldehyde. Electrochemical impedance spectroscopy (EIS) and transient photocurrent measurements demonstrated the semiconducting behavior of CZ-DCM. Subsequently, the Friedel−Crafts reaction of CZ-DCM with octavinylsilsesquioxane (OVS) was carried out to prepare a novel hybrid network (PCS-CZ-DCM) with a high surface area of 954 m 2 g −1 and a large pore volume of 0.96 cm 3 g −1 , which also showed semiconducting behavior. PCS-CZ-DCM exhibited a regulatable near-IR-luminescence sensitivity to berberine chloride hydrate (BCH), which was not influenced by other antibiotics. It displayed a good pH stability ranging from 2 to 11, and the fluorescence quenching constant K SV was 2.1 × 10 4 M −1 . Moreover, PCS-CZ-DCM exhibited excellent photodegradation activity for antibiotics without additional oxidation agents or pH adjustments. PCS-CZ-DCM was highly stable and can be easily regenerated. After seven cycles, the removal rate was still maintained as high as 85%. Thus, we realized concurrent detection and degradation of BCH. ESR analysis proved that the superoxide radical (•O 2 − ) had a significant impact on the photocatalytic system of PCS-CZ-DCM. The outstanding results using PCS-CZ-DCM demonstrated its potential for the control of antibiotic pollutants in environmental applications.

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“…To date, varied types of MOF-hybridized composites have been investigated for their applications in fields with various functions, such as gas adsorption, 21 , 22 sterilization, 23 , 24 and photocatalytic activity. 25 , 26 However, the research studies based on MOF-hybridized composites are mostly focused on exploring the conditions under which the maximum photodegradation and adsorption were achieved, rather than analyzing the individual contribution to the total removal capability. 26 − 28 Also, the findings from previous studies on the effect of environmental conditions (pH, contaminant types, etc.)…”

Section: Introductionmentioning

confidence: 99%

MIL-100(Fe)-Hybridized Nanofibers for Adsorption and Visible Light Photocatalytic Degradation of Water Pollutants: Experimental and DFT Approach

Lee

Ahn

et al. 2022

ACS Omega

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As rapid industrial growth spawns severe water contamination and a far-reaching impact on environmental safety, the development of a purification system is in high demand. Herein, a visible light-induced photocatalytic adsorbent membrane was developed by growing a porous metal–organic framework (MOF), MIL-100(Fe) crystals, onto electrospun polyacrylonitrile (PAN) nanofibers, and its purification capability by adsorption and the photocatalytic effect was investigated. As water-soluble organic foulants, a cationic dye, rhodamine B (RhB), and an anionic dye, methyl orange (MO), were employed, and the adsorption/desorption characteristics were analyzed. Since MIL-100(Fe) possesses positive charges in aqueous solution, MO was more rapidly adsorbed onto the MIL-100(Fe) grown PAN membrane (MIL-100(Fe)@PAN) than RhB. Under visible light, both photocatalytic degradation and adsorption occurred concurrently, facilitating the purification process. The reusability of MIL-100(Fe)@PAN as an adsorbent was explored by cyclic adsorption–desorption experiments. Density functional theory (DFT) calculations corroborated higher binding energy of charged MO over RhB and demonstrated the possible steric hindrance of RhB to adhere in MOF pores. The emphasis of the study lies in the combined investigation of the experimental approach and DFT calculations for the fundamental understanding of adsorption/desorption phenomena occurring in the purification process. This study provides theoretical support for the interaction between MOF–hybrid complexes and contaminants when MOF-hybridized composites adsorb or photodegrade water-soluble pollutants of different charges and sizes.

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Porphyrin-Based Two-Dimensional Layered Metal–Organic Framework with Sono-/Photocatalytic Activity for Water Decontamination

Cited by 100 publications

References 79 publications

Promoted Type I and II ROS Generation by a Covalent Organic Framework through Sonosensitization and PMS Activation

Promoted Type I and II ROS Generation by a Covalent Organic Framework through Sonosensitization and PMS Activation

Organic–Inorganic Hybrid Near-Infrared Emitting Porous Polymer for Detection and Photodegradation of Antibiotics

MIL-100(Fe)-Hybridized Nanofibers for Adsorption and Visible Light Photocatalytic Degradation of Water Pollutants: Experimental and DFT Approach

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