Metalloporphyrin-based D-A type conjugated organic polymer nanotube for efficient photocatalytic degradation

Jun, Han; Zhu, Zhi‐Jun; Li, Najun; Chen, Dongyun; Xu, Qingfeng; Li, Hua; He, Jinghui; Lu, Jianmei

doi:10.1016/j.apcatb.2021.120108

Cited by 79 publications

(28 citation statements)

References 66 publications

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“…The UV light can co-stimulate the LCCT and MLCT transitions in MOF-525-Fe/Zr, which further improves the migration rate of photoelectrons, inhibiting the recombination of photoelectron-hole pairs. LCCT and MLCT effectively reduce the charge transfer resistance, and improve the carrier density and optical stability [57,58].…”

Section: Analysis Of Photoelectric Propertiesmentioning

confidence: 99%

Reconstruction of Electronic Structure of MOF-525 via Metalloporphyrin for Enhanced Photoelectro-Fenton Process

Han

Lin

et al. 2022

Catalysts

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Photoelectro-Fenton (PEF) process can continuously promote the occurrence of Fenton reaction and the generation of active species, which is an advanced oxidation technology for pollutant degradation. However, the lack of bifunctional catalysts restricts the development of PEF technology. In this study, the electronic rearrangement MOF-525 modified by metalloporphyrin (named MOF-525-Fe/Zr) was prepared, to load on the carbon felt as a novel cathode catalyst, which is used in PEF process. A series of characterization and photoelectric chemical properties tests combined with DFT calculation showed that the modification of MOF-525 could not only have the large specific surface area and multistage pore structure but also co-stimulate the metal-to-ligand charge transfer (MLCT) and ligand-to-cluster charge transfer (LCCT) by photoelectric synergy. These charge transitions provide periodic electron donor-acceptor conduction paths in MOF-525-Fe/Zr, which can improve the active species formation and transfer efficiency. Owing to their favorable pore and electronic structure as well as stability, MOF-525-Fe/Zr shows great promise for the application in the catalytic process of PEF. Sulfamethoxazole (SMX) degradation was enhanced by MOF-525-Fe/Zr with the TOC removal rate above 75% both in river water and tap water. Finally, the reasonable pathway of PEF catalytic degradation of SMX was proposed by HPLC-MS analysis. In conclusion, this study provides a new idea for reconstructing the electronic structure of MOFs catalyst and broadening the practical application of PEF technology.

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Section: Analysis Of Photoelectric Propertiesmentioning

confidence: 99%

Reconstruction of Electronic Structure of MOF-525 via Metalloporphyrin for Enhanced Photoelectro-Fenton Process

Han

Lin

et al. 2022

Catalysts

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“…Wang et al reported a side chain extended-conjugation strategy to expand the πconjugated system along both backbone and side chain directions, 12 which strengthens the interchain π−π interactions, thus improving charge mobility and transport. Han et al synthesized porphyrin-based CP nanotubes, 13 where the separation and transfer of photoinduced carriers are improved through the metal-to-ligand charge transfer and electron push− pull effect between porphyrin units and benzothiadiazole moieties.…”

Section: Introductionmentioning

confidence: 99%

Rational Design of Alkynyl-Based Linear Donor−π–Acceptor Conjugated Polymers with Accelerated Exciton Dissociation for Photocatalysis

Xiao

et al. 2022

Macromolecules

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Boosting the slow exciton dissociation of conjugated polymers (CPs) is of significance for their application in photocatalysis. Extensive research has been dedicated to improve the exciton separation efficiency through the rational molecular design, while constructing donor−π–acceptor (D−π–A) structures with larger π-electron delocalization to extend carrier migrating distance can further promote exciton dissociation. In this work, we reported the design and construction of D−π–A CP systems by using pyrene, dibenzo[b,d]thiophene 5,5-dioxide, and diethynylbenzene as the donor group, acceptor group, and π-linker units, respectively, for improving the photocatalytic performance. Density functional theory studies and experimental investigations reveal that the D−π–A structure can suppress charge recombination, minimize exciton binding energy, and extend the light absorption range, thereby improving the photocatalytic activity in comparison to the A−π–A and D−π–D structures. It is believed that this work can provide inspiration for the precise regulation of the D−π–A system by combining experiments and theoretical calculations, thereby enhancing the photocatalytic performance of CPs.

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“…13 At present, in order to improve the separation of photogenerated carriers on the COF surface, increase the migration speed of electrons and shorten the migration distance of carriers, researchers have proposed methods such as constructing D (donor)-A (acceptor) structures and modifying the monomer structure. [14][15][16] These strategies mainly use the push-pull effect of electrons to control the separation of photogenerated carriers. However, these strategies are insufficient for developing efficient photocatalytic hydrogen evolution COFs.…”

Section: Introductionmentioning

confidence: 99%

Identifying the roles of imine and alkyne linkages in determining the photocatalytic hydrogen evolution over thiadiazole-based covalent organic frameworks

et al. 2022

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Metalloporphyrin-based D-A type conjugated organic polymer nanotube for efficient photocatalytic degradation

Cited by 79 publications

References 66 publications

Reconstruction of Electronic Structure of MOF-525 via Metalloporphyrin for Enhanced Photoelectro-Fenton Process

Reconstruction of Electronic Structure of MOF-525 via Metalloporphyrin for Enhanced Photoelectro-Fenton Process

Rational Design of Alkynyl-Based Linear Donor−π–Acceptor Conjugated Polymers with Accelerated Exciton Dissociation for Photocatalysis

Identifying the roles of imine and alkyne linkages in determining the photocatalytic hydrogen evolution over thiadiazole-based covalent organic frameworks

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