Leveraging doping and defect engineering to modulate exciton dissociation in graphitic carbon nitride for photocatalytic elimination of marine oil spill

Xia, Linhong; Sun, Zhaoli; Wu, Yu‐Ning; Yu, Xing; Cheng, Jianbo; Zhang, Kaisheng; Sarina, Sarina; Zhu, Hongkai; Weerathunga, Helapiyumi; Zhang, Lixue; Xia, Jianfei; Yu, Jianqiang; Yang, Xiaolong

doi:10.1016/j.cej.2022.135668

Cited by 52 publications

(18 citation statements)

References 61 publications

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“…34−36 The intensity of the EPR signal of CN-P-3 was much stronger than that of CN, which was attributed to the redistribution of electrons within the CN-P-3 structure by the electron donation from the phosphorus species and the existence of carbon vacancies. 15,37,26 X-ray photoelectron spectroscopy (XPS) confirmed that P atoms replaced C atoms and generated carbon vacancies (Figures S7b,c and S8). The optical properties of all samples were measured by UV−vis diffuse reflectance spectroscopy.…”

Section: Resultsmentioning

confidence: 97%

“…The EPR spectra were used to further study the unpaired electrons in the samples (Figure f). CN and CN-P-3 exhibited strong signals with centers around 3512 G, which was attributed to the unpaired electrons within the π-conjugated aromatic rings of sp 2 -carbon. − The intensity of the EPR signal of CN-P-3 was much stronger than that of CN, which was attributed to the redistribution of electrons within the CN-P-3 structure by the electron donation from the phosphorus species and the existence of carbon vacancies. ,, …”

Section: Resultsmentioning

confidence: 99%

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In Situ Construction of an Intramolecular Donor–Acceptor Conjugated Copolymer via Terephthalic Acid Derived from Plastic Waste for Photocatalysis of Plastic to Hydrogen Peroxide

Gong,

Ma,

Zhang

et al. 2023

ACS Catal.

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Photocatalysis offers promising technology for converting plastic waste into valuable chemicals. However, fully digging out the embedded value to incentivize the valorization of plastic waste is still a challenge. Herein, we first design an intramolecular donor–acceptor (D–A) structure by introducing the terephthalic acid (PTA) derived from polyethylene terephthalate (PET) waste into P-doped g-C3N4 (CN-P). Impressively, CN-P-PTA exhibits higher activity in the photocatalysis of PET to H2O2 compared with CN-P. The superior performance is attributed to the prolonged photogenerated carrier lifetime and the enhanced delocalization of π electrons. Moreover, single-particle PL quenching and DFT calculations reveal that PTA and CN-P can form an intimate interface via π–π conjugation, which facilitates the flow of photoexcited electrons from PTA to CN-P.

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Section: Resultsmentioning

confidence: 97%

Section: Resultsmentioning

confidence: 99%

In Situ Construction of an Intramolecular Donor–Acceptor Conjugated Copolymer via Terephthalic Acid Derived from Plastic Waste for Photocatalysis of Plastic to Hydrogen Peroxide

Gong,

Ma,

Zhang

et al. 2023

ACS Catal.

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“…Within the realm of elemental doping modifications for g-C 3 N 4 , the substitution doping with non-metallic elemental oxygen (O) has exhibited particularly promising outcomes. 25 Substitution of elements C, N and H by O in the 3s-triazine structural unit of g-C 3 N 4 can change the charge distribution and symmetry of g-C 3 N 4 26 and optimized material primitive reaction steps, 27 which improving the separation and utilization efficiency of photogenerated carriers in carbon nitride. 28 This ultimately leads to improved photocatalytic performance.…”

Section: Introductionmentioning

confidence: 99%

Oxygen-Doped Porous g-C₃N₄ via Oxalic Acid-Assisted Thermal Polycondensation as a Visible Light-Driven Photocatalyst for Bisphenol A Degradation

Wei,

Liu,

Liu

et al. 2023

ACS Appl. Nano Mater.

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Graphitic phase carbon nitride (g-C3N4) demonstrates tremendous potential for photocatalytic degradation of organic pollutants, but its performance is severely limited by the high recombination of photogenerated electron–hole pairs. This study introduces an innovative approach oxalic acid-assisted thermal polycondensation to construct a series of oxygen-doped porous g-C3N4 (OCN) nanostructured materials, which simultaneously utilizes the heat-induced foaming mechanism of oxalic acid to achieve element doping modification. The results indicate that modified OCN-1.5 exhibited the optimal photocatalytic activity. Under visible light conditions, the degradation efficiency of OCN-1.5 catalyst toward bisphenol A (BPA, 30 mg L–1) reached 82.55% (240 min light irradiation). This represents a significant improvement of 60% compared to the traditional g-C3N4 catalyst. The mechanism is as follows: on the one hand, the doping of oxygen atoms alter the charge distribution and symmetry of g-C3N4, thereby enhancing the separation efficiency of photogenerated charge carriers. Furthermore, under visible light irradiation, it facilitates the formation of conjugated delocalized systems associated with e– and h+ on the surface, leading to an accelerated mineralization degradation of OCN and BPA at the interface. Additionally, the •O2 – radicals generated from the interfacial reactions can also directly oxidize BPA simultaneously. On the other hand, the construction of a porous nanostructure provides a larger specific surface area and channels for the diffusion of charge carriers, thereby enhancing light capture and transfer. Moreover, this structure offers more active sites for the adsorption and degradation of pollutants. Therefore, the synthetic strategy proposed in this study overcomes the long-standing aggregation issue in the synthesis of g-C3N4, providing a perspective for the scalable preparation of high-performance g-C3N4 photocatalysts and the removal of organic pollutants.

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“…However, the photoexcitation process of bulk carbon nitride prepared by nitrogen-containing precursors such as melamine generates a large number of Frenkel excitons [17,21]. The strong Coulomb force between Frenkel excitons in bulk g-C 3 N 4 leads to high exciton binding energy, resulting in slow exciton dissociation and severe charge recombination, which is unfortunately often overlooked [22]. Besides, the stacked sheet structure of bulk carbon nitride results in low specific surface area and insufficient reaction sites, which significantly impairs the photocatalytic performance of carbon nitride [12,16,23].…”

Section: Introductionmentioning

confidence: 99%

Boron nitride quantum dots modified carbon-defects ultra-thin porous carbon nitride: double channels and quantum size effects facilitate photogenerated carrier migration and exciton dissociation

Huang

Jiang

2023

Mater. Res. Express

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Graphite carbon nitride possesses great promise for visible photocatalysis, but the bulk carbon nitride prepared from nitrogen-rich precursors such as melamine has inherent drawbacks such as retarded photogenerated carrier migration and exciton effects, which limit its application. Herein, we constructed a novel Boron nitride quantum dots modified carbon-defects ultra-thin porous carbon nitride (BNQDs/Vc-UPCN). The double channels were constructed by carbon-defects structure and Boron nitride quantum effect to overcome its inherent drawbacks and applied to the photodegradation of common persistent organic pollutants (methylene blue). The structure, porosity, elemental composition, optical properties, photoelectrochemical properties, and photocatalytic properties of the prepared BNQDs/Vc-UPCN composites were investigated using various characterization methods. Meanwhile, the results of radical trapping experiments and electron spin resonance characterization demonstrated that BNQDs/Vc-UPCN promote molecular oxygen activation more than Vc-UPCN did. In terms of degradation effect, the best sample (BC-1) is 10 times more effective than the initial sample (BCN). This study proposes an effective mechanism for constructing novel visible-light-driven photocatalysts using carbon-defects ultra-thin structures and quantum dots, which can be used for the treatment of organic pollutants.

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Leveraging doping and defect engineering to modulate exciton dissociation in graphitic carbon nitride for photocatalytic elimination of marine oil spill

Cited by 52 publications

References 61 publications

In Situ Construction of an Intramolecular Donor–Acceptor Conjugated Copolymer via Terephthalic Acid Derived from Plastic Waste for Photocatalysis of Plastic to Hydrogen Peroxide

In Situ Construction of an Intramolecular Donor–Acceptor Conjugated Copolymer via Terephthalic Acid Derived from Plastic Waste for Photocatalysis of Plastic to Hydrogen Peroxide

Oxygen-Doped Porous g-C₃N₄ via Oxalic Acid-Assisted Thermal Polycondensation as a Visible Light-Driven Photocatalyst for Bisphenol A Degradation

Boron nitride quantum dots modified carbon-defects ultra-thin porous carbon nitride: double channels and quantum size effects facilitate photogenerated carrier migration and exciton dissociation

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Leveraging doping and defect engineering to modulate exciton dissociation in graphitic carbon nitride for photocatalytic elimination of marine oil spill

Cited by 52 publications

References 61 publications

In Situ Construction of an Intramolecular Donor–Acceptor Conjugated Copolymer via Terephthalic Acid Derived from Plastic Waste for Photocatalysis of Plastic to Hydrogen Peroxide

In Situ Construction of an Intramolecular Donor–Acceptor Conjugated Copolymer via Terephthalic Acid Derived from Plastic Waste for Photocatalysis of Plastic to Hydrogen Peroxide

Oxygen-Doped Porous g-C3N4 via Oxalic Acid-Assisted Thermal Polycondensation as a Visible Light-Driven Photocatalyst for Bisphenol A Degradation

Boron nitride quantum dots modified carbon-defects ultra-thin porous carbon nitride: double channels and quantum size effects facilitate photogenerated carrier migration and exciton dissociation

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Product

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Oxygen-Doped Porous g-C₃N₄ via Oxalic Acid-Assisted Thermal Polycondensation as a Visible Light-Driven Photocatalyst for Bisphenol A Degradation