Exfoliation-induced O-doped g-C3N4 nanosheets with improved photoreactivity towards RhB degradation and H2 evolution

Yan, Juntao; Liu, Jinhong; Sun, Yuekai; Ding, Deng; Wang, Chunlei; Sun, Lin; Li, Xiaofang

doi:10.1039/d1qi01625c

Cited by 29 publications

(12 citation statements)

References 49 publications

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“…situ plasma synthesis strategy also shows a high apparent quantum yield (AQY) of 4.14% at 450 nm, which is close to industrial utility [33]. With the help of theoretical calculation, we believe the improvement of hydrogen production performance of photocatalysts prepared by the plasma method is due to the favorable hydrophilic sites [34,35] and rearranged electronic structure [36,37] caused by carboxyl defects (Figure 8). The carboxyl defect sites may also promote the binding state of Pt cocatalysts for H2 generation.…”

Section: Visible-light-driven H 2 Evolution Performances and Optimiza...mentioning

confidence: 73%

“…As a result, more active sites for hydrogen production were developed, and thus both the H2O to H2 reaction and the H + to H2 reaction were boosted, leading to the superior H2 evolution performance. Based on the above experimental results, we believe that the plasma modification strategy proposed in this paper can effectively control the defect structure and electronic With the help of theoretical calculation, we believe the improvement of hydrogen production performance of photocatalysts prepared by the plasma method is due to the favorable hydrophilic sites [34,35] and rearranged electronic structure [36,37] caused by carboxyl defects (Figure 8). The carboxyl defect sites may also promote the binding state of Pt cocatalysts for H 2 generation.…”

Section: Visible-light-driven H 2 Evolution Performances and Optimiza...mentioning

confidence: 82%

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H2+CO2 Synergistic Plasma Positioning Carboxyl Defects in g-C3N4 with Engineered Electronic Structure and Active Sites for Efficient Photocatalytic H2 Evolution

Wang

Zhang

et al. 2022

IJMS

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Defective functional-group-endowed polymer semiconductors, which have unique photoelectric properties and rapid carrier separation properties, are an emerging type of high-performance photocatalyst for various energy and environmental applications. However, traditional oxidation etching chemical methods struggle to introduce defects or produce special functional group structures gently and controllably, which limits the implementation and application of the defective functional group modification strategy. Here, with the surface carboxyl modification of graphitic carbon nitride (g-C3N4) photocatalyst as an example, we show for the first time the feasibility and precise modification potential of the non-thermal plasma method. In this method, the microwave plasma technique is employed to generate highly active plasma in a combined H2+CO2 gas environment. The plasma treatment allows for scalable production of high-quality defective carboxyl group-endowed g-C3N4 nanosheets with mesopores. The rapid H2+CO2 plasma immersion treatment can precisely tune the electronic and band structures of g-C3N4 nanosheets within 10 min. This conjoint approach also promotes charge-carrier separation and accelerates the photocatalyst-catalyzed H2 evolution rate from 1.68 mmol h−1g−1 (raw g-C3N4) to 8.53 mmol h−1g−1 (H2+CO2-pCN) under Xenon lamp irradiation. The apparent quantum yield (AQY) of the H2+CO2-pCN with the presence of 5 wt.% Pt cocatalyst is 4.14% at 450 nm. Combined with density functional theory calculations, we illustrate that the synergistic N vacancy generation and carboxyl species grafting modifies raw g-C3N4 materials by introducing ideal defective carboxyl groups into the framework of heptazine ring g-C3N4, leading to significantly optimized electronic structure and active sites for efficient photocatalytic H2 evolution. The 5.08-times enhancement in the photocatalytic H2 evolution over the as-developed catalysts reveal the potential and maneuverability of the non-thermal plasma method in positioning carboxyl defects and mesoporous morphology. This work presents new understanding about the defect engineering mechanism in g-C3N4 semiconductors, and thus paves the way for rational design of effective polymeric photocatalysts through advanced defective functional group engineering techniques evolving CO2 as the industrial carrier gas.

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Section: Visible-light-driven H 2 Evolution Performances and Optimiza...mentioning

confidence: 73%

Section: Visible-light-driven H 2 Evolution Performances and Optimiza...mentioning

confidence: 82%

H2+CO2 Synergistic Plasma Positioning Carboxyl Defects in g-C3N4 with Engineered Electronic Structure and Active Sites for Efficient Photocatalytic H2 Evolution

Wang

Zhang

et al. 2022

IJMS

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“…In addition, introducing other non-metal elements are also effective strategies in promoting the photocatalytic property (Deng et al, 2019;Li et al, 2021b;Li et al, 2021c;Liu et al, 2021;Yan et al, 2022). For instance, carbon (C) self-doped g-C 3 N 4 was prepared via a combined method of melaminecyanuric acid complex supramolecular pre-assembly and solvothermal pre-treatment (Li et al, 2021b).…”

Section: Non-metal Dopingmentioning

confidence: 99%

“…The H 2 evolution rate for optimized g-C 3 N 4 was 18 times higher than that of bulk g-C 3 N 4 , and the enhanced performance derives from the extended optical absorption, accelerated photoactivated charge carrier separation, and transfer efficiency. Unique oxygen-doped g-C 3 N 4 materials were synthesized, which realized the synergetic control of the electronic structure and morphology and possessed the advantages of enlarged surface area, increased exposed active edges, and improved separation efficiency (Yan et al, 2022). Some other high-performance nonmetal doped materials including phosphorus-doped g-C 3 N 4 (Yang et al, 2018;Lin et al, 2020;Zhao et al, 2020) and sulfur-doped g-C 3 N 4 (Li et al, 2019a;Yang et al, 2020b;Long et al, 2020) have also been developed.…”

Section: Non-metal Dopingmentioning

confidence: 99%

Recent Progress in Doped g-C3N4 Photocatalyst for Solar Water Splitting: A Review

et al. 2022

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Graphitic carbon nitride (g-C3N4) photocatalysis for water splitting is harvested as a fascinating way for addressing the global energy crisis. At present, numerous research subjects have been achieved to design and develop g-C3N4 photocatalysis, and the photocatalytic system still suffers from low efficiency that is far from practical applications. Here, there is an inspiring review on the latest progress of the doping strategies to modify g-C3N4 for enhancing the efficiency of photocatalytic water splitting, including non-metal doping, metal doping, and molecular doping. Finally, the review concludes a summary and highlights some perspectives on the challenges and future research of g-C3N4 photocatalysts.

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“…[4] Converting inexhaustible solar energy into clean and stored hydrogen has been the focus of recent research. [5][6][7] The main task at this stage searches for highly efficient catalysts from non-noble metals and combine them with highly active photosensitizers (PS) into a reliable system for hydrogen production. [8,9] In recent years, it has been found that the photocatalysts, composed of transition metal complexes such as Fe, Co and Ni, are beneficial to the absorption of electrons because they have unfilled orbitals and can be used as separation centers for photogenerated electrons and holes, thus improving the activity of hydrogen production.…”

Section: Introductionmentioning

confidence: 99%

Photocatalytic Hydrogen Production Activity and Mechanism of New Nickel‐Based Sulfur Complexes in Aqueous Solution

Shi

Huang

et al. 2023

ChemPhysChem

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The development of industry and the increase in population have caused energy shortages and environmental pollution problems. Developing clean and storable new energy is identified as a key way to solve the problems above. Hydrogen is viewed as the most potential energy carrier due to its high calorific value and pollution‐free. To convert solar energy into hydrogen energy, three nickel‐based catalysts, Ni(aps)(pys)2 (aps=2‐amino‐2‐phenylacetic salicylaldehyde) (1), Ni(ads)(pys)2 (ads=aniline salicylaldehyde, pys=pyridine‐2‐thiolate) (2), Ni(acs)(pys)2 (acs=aniline 5‐chlorosalicylaldehyde) (3), were synthesized and explored as photocatalysts for hydrogen production. A three‐component photocatalytic system for hydrogen production was constructed using target complex as photocatalyst, triethanolamine (TEOA) as electron sacrificial agent and fluorescein (FL) as photosensitizer. Under the optimum conditions, about 1504 μmol of H2 can be obtained with 25 mg catalyst 2 after 3 hours of irradiation. Finally, the hydrogen‐production mechanism was discussed by experimental and theoretical methods.

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Exfoliation-induced O-doped g-C₃N₄ nanosheets with improved photoreactivity towards RhB degradation and H₂ evolution

Abstract: Graphitic carbon nitride (g-C3N4) nanosheets exfoliated from bulk-sized counterparts are limited by quantum size effect-induced widened bandgap. In this work, a (NH4)2S2O8 (APS) induced thermal exfoliation approach is introduced to...

Cited by 29 publications

References 49 publications

H2+CO2 Synergistic Plasma Positioning Carboxyl Defects in g-C3N4 with Engineered Electronic Structure and Active Sites for Efficient Photocatalytic H2 Evolution

H2+CO2 Synergistic Plasma Positioning Carboxyl Defects in g-C3N4 with Engineered Electronic Structure and Active Sites for Efficient Photocatalytic H2 Evolution

Recent Progress in Doped g-C3N4 Photocatalyst for Solar Water Splitting: A Review

Photocatalytic Hydrogen Production Activity and Mechanism of New Nickel‐Based Sulfur Complexes in Aqueous Solution

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