Highly-crystalline Triazine-PDI Polymer with an Enhanced Built-in Electric Field for Full-Spectrum Photocatalytic Phenol Mineralization

Zhang, Hanjie; Chen, Xianjie; Zhang, Zijian; Yu, Kunyi; Wang, Zhu; Zhu, Yongfa

doi:10.1016/j.apcatb.2021.119957

Cited by 96 publications

(31 citation statements)

References 49 publications

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“…Accordingly, an internal electric field induced by the charge distribution can greatly suppress the recombination of photogenerated carriers and improve the photocatalytic H 2 production . Furthermore, based on the built-in electric field characterization method reported by Zhang et al and according to the specific calculation eq S1 described in the supporting materials, open-circuit potential (vs NHE) and zeta potential of the photocatalysts were examined, which represent the surface voltage and surface charge density, respectively, as shown in Figure b. Briefly, the relative built-in electric field intensity can be evaluated by multiplying the value of the open-circuit potential and zeta potential for each catalyst.…”

Section: Resultsmentioning

confidence: 99%

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Molecular Self-Assembly of Oxygen Deep-Doped Ultrathin C₃N₄ with a Built-In Electric Field for Efficient Photocatalytic H₂ Evolution

Zhang

et al. 2021

Inorg. Chem.

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Heteroatom-doped carbon nitride (C 3 N 4 ) with a built-in electric field can reinforce the carrier separation; however, the stability will be greatly reduced due to the loss of surface-doped atoms. Here, molecule self-assembly, as a facile bottom-up approach, is explored for the synthesis and oxygen doping of C 3 N 4 . The obtained C 3 N 4 presents a porous and ultrathin structure and oxygen deep-doping, which generate abundant nitrogen vacancies and a stable built-in electric field. Toward photocatalytic hydrogen evolution, the ultrathin and oxygen deep-doped C 3 N 4 exhibits a 3.5-fold higher activity than bulk C 3 N 4 under simulated sunlight, and 3.6 times higher stability than the oxygen surface-doped counterpart within five cycles. Femtosecond transient absorption spectroscopy indicates the improved carrier separation, and density functional theory (DFT) calculation reveals the promoted H 2 O adsorption and activation under the built-in electric field, which contribute to the excellent photocatalytic performance of oxygen deep-doped ultrathin C 3 N 4 .

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Section: Resultsmentioning

confidence: 99%

Section: Resultsmentioning

confidence: 99%

Molecular Self-Assembly of Oxygen Deep-Doped Ultrathin C₃N₄ with a Built-In Electric Field for Efficient Photocatalytic H₂ Evolution

Zhang

et al. 2021

Inorg. Chem.

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“…Constructing a built-in electric field (BEF) in semiconductors is considered as a viable strategy to boost exciton dissociation into electron–hole pairs to realize the maximum carrier separation in the photocatalytic systems. − In particular, driven by the BEF, the photogenerated holes and electrons will transfer in opposite directions, thus drastically accelerating the separation of excitons. A strong BEF relies on the polarization of semiconductors, which was induced by molecular dipole.…”

Section: Introductionmentioning

confidence: 99%

Enhancing Built-in Electric Field via Molecular Dipole Control in Conjugated Microporous Polymers for Boosting Charge Separation

Deng

Zhao

Cao

et al. 2022

ACS Appl. Mater. Interfaces

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The built-in electric field (BEF) has been considered as the key kinetic factor for facilitating efficient photoinduced carrier separation and migration of polymeric photocatalysts. Enhancing the BEF of the polymers could enable a directional migration of the photogenerated carriers to accelerate photogenerated charge separation and thus boost photocatalytic performances. However, achieving this approach remains a formidable challenge, which has never been realized in conjugated microporous polymers (CMPs). Herein, we developed a molecular dipole control strategy to modulate the BEF in CMPs by varying the nature of the core. As a result, a series of CMPs with a tunable BEF were designed and prepared via FeCl3-mediated coupling of bicarbazole with different acceptor cores. The optimized CbzCMP-9 featured the strongest BEF induced by its high molecular dipole, which grants it with a powerful driving force to accelerate exciton dissociation into electron–hole pairs and facilitates charge transfer along the backbone of CMPs to the surface, resulting in a remarkable photocatalytic performance toward thiocyano chromones and C-3 thiocyanation of indoles (up to 95 and 98% yields, respectively) and prominently surpassing many other reported photocatalysts. In brief, the proposed strategy highlights that enhancing the BEF by modulating molecular dipole can lead to a dramatic improvement in photocatalytic performance, which is expected to be employed for constructing other photocatalytic systems with high performance.

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“…Semiconductor photocatalysts have attracted tremendous attention due to their great potential in promoting light-driven reactions associated with energy conversion − and contaminant treatment. − Unfortunately, when materials shrink from bulk to smaller size or dimensionality, they show strong excitonic effects (the Coulombic interaction of electron–hole pairs), − causing the quick recombination and annihilation of electron–hole pairs, significantly restricting charge carrier (excited electron and hole) transfer, and impeding the generation of reactive oxygen species (ROS). , Notably, recombination of electron–hole pairs typically finishes within a few picoseconds, much faster than photoinduced charge carrier separation and photocatalytic reactions . This is the dominant limiting step to achieve satisfactory photocatalytic performance .…”

Section: Introductionmentioning

confidence: 99%

CdTe Quantum Dot/Bi₂WO₆ Nanosheet Photocatalysts with a Giant Built-In Electric Field for Enhanced Removal of Persistent Organic Pollutants

Yang

Zhang

Chen

et al. 2022

ACS Appl. Nano Mater.

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Constrained by the strong Coulombic interaction of electron–hole pairs in semiconductor photocatalysts, the charge carrier separation and the resultant photocatalytic capability are greatly compromised. In this work, we rationally construct a built-in electric field (BEF) from the (111) facet of CdTe quantum dots (CdTeQDs) to the (200) facet of two-dimensional Bi2WO6 (2DBWO) nanosheets by the formation of a Te–O x bond. We validate experimentally and theoretically that the BEF can profoundly promote the dissociation of a photoexcited exciton and separation of a charge carrier, resulting in the formation of a Z-scheme electronic structure of the CdTeQDs/2DBWO photocatalyst. Benefiting from the role of the BEF, the photoinduced generation of the superoxide anion radical and hydroxyl radical is significantly promoted, based on which photodegradation performances of the CdTeQDs/2DBWO photocatalyst are 6.64, 1.95, and 5.4 times those of pure 2DBWO for tetracycline, phenol, and rhodamine B, respectively. This work provides a mechanistic insight into the design and optimization of semiconductor heterojunction photocatalysts for efficient charge carrier separation and environmental remediation.

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Highly-crystalline Triazine-PDI Polymer with an Enhanced Built-in Electric Field for Full-Spectrum Photocatalytic Phenol Mineralization

Cited by 96 publications

References 49 publications

Molecular Self-Assembly of Oxygen Deep-Doped Ultrathin C₃N₄ with a Built-In Electric Field for Efficient Photocatalytic H₂ Evolution

Molecular Self-Assembly of Oxygen Deep-Doped Ultrathin C₃N₄ with a Built-In Electric Field for Efficient Photocatalytic H₂ Evolution

Enhancing Built-in Electric Field via Molecular Dipole Control in Conjugated Microporous Polymers for Boosting Charge Separation

CdTe Quantum Dot/Bi₂WO₆ Nanosheet Photocatalysts with a Giant Built-In Electric Field for Enhanced Removal of Persistent Organic Pollutants

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Highly-crystalline Triazine-PDI Polymer with an Enhanced Built-in Electric Field for Full-Spectrum Photocatalytic Phenol Mineralization

Cited by 96 publications

References 49 publications

Molecular Self-Assembly of Oxygen Deep-Doped Ultrathin C3N4 with a Built-In Electric Field for Efficient Photocatalytic H2 Evolution

Molecular Self-Assembly of Oxygen Deep-Doped Ultrathin C3N4 with a Built-In Electric Field for Efficient Photocatalytic H2 Evolution

Enhancing Built-in Electric Field via Molecular Dipole Control in Conjugated Microporous Polymers for Boosting Charge Separation

CdTe Quantum Dot/Bi2WO6 Nanosheet Photocatalysts with a Giant Built-In Electric Field for Enhanced Removal of Persistent Organic Pollutants

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Molecular Self-Assembly of Oxygen Deep-Doped Ultrathin C₃N₄ with a Built-In Electric Field for Efficient Photocatalytic H₂ Evolution

Molecular Self-Assembly of Oxygen Deep-Doped Ultrathin C₃N₄ with a Built-In Electric Field for Efficient Photocatalytic H₂ Evolution

CdTe Quantum Dot/Bi₂WO₆ Nanosheet Photocatalysts with a Giant Built-In Electric Field for Enhanced Removal of Persistent Organic Pollutants