Effective modification of photocatalytic and piezocatalytic performances for poly(heptazine imide) by carbon dots decoration

Wang, Shijie; Zhang, Haoqing; Nie, Ran; Ning, Yuxin; Zhao, Chenxi; Xia, Zhonghui; Niu, Ping; Li, Li; Wang, Shulan

doi:10.1039/d2dt01819e

Cited by 9 publications

(7 citation statements)

References 61 publications

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“…In Figure S6d, Supporting Information, C 1s spectra exhibited five deconvoluted peaks at around 284.8, 286.6, 287.9, 289.5, and 294 eV, which can be assigned to C─C, C─N, N═C─N, O═C─O, and π─π* bonds, respectively, in the materials. [36][37][38] The high-resolution spectra of N 1s in Figure S6e, Supporting Information reveal the presence of C═N─C, N─(C) 3 , C─N─H, and π─π* bonds. While these peaks for ICN were located at 398.8, 400, 400.9, and 404.6 eV, the shifting to higher binding energy was observed for ACN and CN, with these peaks being situated at 399.9, 401.6, 402.3, and 405.9 eV, respectively.…”

Section: Resolving Catalyst's Structuresmentioning

confidence: 99%

Unraveling Precise Locations of Indium Atoms in g‐C₃N₄ for Ameliorating Hydrogen Peroxide Piezo‐Photogeneration

Anh,

Nguyen,

Luu

et al. 2024

Solar RRL

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Increasing active sites in catalysts is of utmost importance for catalytic processes. In this regime, single‐atom dispersing on graphitic carbon nitrides (g‐C3N4) to produce fine chemicals, such as hydrogen peroxide (H2O2), is of current interest due to not only enhancing catalytic performance but also reducing the loading of necessary metals. Hence, we, in this research, engineered g‐C3N4 by atomically dispersing aluminum (Al) or indium (In) sites to provide catalytic active centers via one‐step thermal shock polymerization. The addition of Al and In sites can accelerate the catalytic efficacy owing to the Lewis acid‐base interactions between these metals and oxygen (O2). Under catalytic conditions, the formation of oxygenic radicals would strongly be associated with the enhanced formation of H2O2, confirmed by in‐situ electron paramagnetic resonance (EPR) spectroscopy. Furthermore, the empirical analyses from positron annihilation spectroscopy (PAS) show that In atoms would occupy the near positions of carbon vacancies (VC) to form N‐VC@In‐O bonds. This replacement would produce the highest formation energy based on the density functional theory (DFT) calculations, improving the stability of atom‐dispersive materials. Therefore, via the combination of experimental and theoretical proofs, this study suggests the exact location of In atoms in g‐C3N4 structures, which can help boost the catalytic production of H2O2.This article is protected by copyright. All rights reserved.

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Section: Resolving Catalyst's Structuresmentioning

confidence: 99%

Unraveling Precise Locations of Indium Atoms in g‐C₃N₄ for Ameliorating Hydrogen Peroxide Piezo‐Photogeneration

Anh,

Nguyen,

Luu

et al. 2024

Solar RRL

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“…In Figure S1g (Supporting Information), the high‐resolution C 1s XPS spectra were dictated with the materials containing five deconvolution peaks at about 284.6, 287.2, 287.5, 287.9, and 293.1 eV, corresponding to C─C, C─N, N═C─N, O═C─O, and π – π * , respectively. [ 33,34 ] Figure S1h (Supporting Information) demonstrates the deconvoluted peaks of N 1s spectra, containing ‐C = N‐C, N─C 3 , C─N─H, and π‐ ‐ π * in the systems. [ 35,36 ] The peak from N 1s spectra without deconvolutions of FCN, CCN, and BCN exhibit the right shift to a lower binding energy region, proving the modified systems gain more free electrons than the pristine CN, improving catalytic outcomes.…”

Section: Resultsmentioning

confidence: 99%

Insights into Molten Salts Induced Structural Defects in Graphitic Carbon Nitrides for Piezo‐Photocatalysis with Multiple H₂O₂ Production Channels

Ly,

Nguyen,

Luu

et al. 2023

Advanced Sustainable Systems

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Elucidating the impact of heteroatoms in graphitic carbon nitrides (g‐C3N4) is of utmost importance to rationalize materials. Hence, in this study, oxygen‐doped g‐C3N4 containing trace amounts of halogen in the structures for piezo‐photosynthesis of hydrogen peroxides (H2O2) is fabricated. The findings reveal that oxygen atoms may be inserted into g‐C3N4 in‐plane structures, while halogen atoms tend to become intercalated between g‐C3N4 layers. Furthermore, the presence of ammonium molten salts (NH4X) during the synthesis alters the concentration of mono and cluster vacancies of carbon and nitrogen in the materials, certifying by positron annihilation spectroscopy (PAS). These defective contributions will be meaningfully accelerate catalytic performance by providing trapping states. Additionally, the decomposition of generated H2O2 can produce highly oxidative hydroxyl radicals, inducing degradations on the catalyst's structures and unexpectedly decreasing catalytic outcomes. From the mechanistic view, different reduction and oxidation channels will be play a pivotal role in generating H2O2. Moreover, the influence of ultrasound and light is also carefully investigated in the work to gain more insights into how the catalysts are triggered to improve catalytic performance. Thus, this study highlights the importance of carefully characterizing structures of g‐C3N4 to precisely understand the catalytic properties, benefiting catalytic design and development.

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“…S6a, the survey spectra display the presence of carbon, nitrogen, and oxygen. Additionally, the unobservable features of Al 2p and In 3d on the survey spectra indicate a very high level of metal dispersion on the g-C 3 N 4 surfaces [31]. The high-resolution XPS spectra of Al 2p and In 3d are depicted in Fig.…”

Section: Resolving Catalyst's Structuresmentioning

confidence: 95%

Unraveling Precise Locations of Indium Atoms in g-C3N4 for Ameliorating Hydrogen Peroxide Piezo-Photogeneration

Vuong,

Anh,

Nguyen

et al. 2023

Preprint

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Increasing active sites in catalysts is of utmost importance for catalytic processes, frequently fascinating global scientists. In recent years, using graphitic carbon nitrides (g-C3N4) for the piezo-photocatalytic generation of fine chemicals, such as hydrogen peroxide (H2O2) from oxygen (O2) and water (H2O), is of current interest due to its flexibility in molecular structures to boost catalytic properties. However, due to its intrinsic nature, bulk g-C3N4 suffers from low catalytic outcomes. To enhance catalytic performances, we, in this research, engineered g-C3N4 by atomically dispersing aluminum (Al) or indium (In) sites to provide catalytic active centers via one-step thermal shock polymerization. The empirical analyses show that In atoms would occupy the near positions of carbon vacancies (VC) to form N-VC@In-O bonds. This replacement would produce the highest formation energy based on the theoretical calculations, improving the stability of atom-dispersive materials. In addition, under catalytic conditions, the formation of oxygenic radicals would strongly be associated with the enhanced formation of H2O2. Unhappily, hydroxyl radicals would induce catalytic deactivation due to the attacks of these highly oxidative radicals on the active centers, thus changing the catalysts' structures and reducing the catalytic outcomes.

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Effective modification of photocatalytic and piezocatalytic performances for poly(heptazine imide) by carbon dots decoration

Abstract: As the high-crystalline phase of carbon nitride, the poly(heptazine imide) (PHI) has attracted much attention in recent years considering its more effective light absorption, better charge carrier behaviors and higher...

Cited by 9 publications

References 61 publications

Unraveling Precise Locations of Indium Atoms in g‐C₃N₄ for Ameliorating Hydrogen Peroxide Piezo‐Photogeneration

Unraveling Precise Locations of Indium Atoms in g‐C₃N₄ for Ameliorating Hydrogen Peroxide Piezo‐Photogeneration

Insights into Molten Salts Induced Structural Defects in Graphitic Carbon Nitrides for Piezo‐Photocatalysis with Multiple H₂O₂ Production Channels

Unraveling Precise Locations of Indium Atoms in g-C3N4 for Ameliorating Hydrogen Peroxide Piezo-Photogeneration

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Effective modification of photocatalytic and piezocatalytic performances for poly(heptazine imide) by carbon dots decoration

Abstract: As the high-crystalline phase of carbon nitride, the poly(heptazine imide) (PHI) has attracted much attention in recent years considering its more effective light absorption, better charge carrier behaviors and higher...

Cited by 9 publications

References 61 publications

Unraveling Precise Locations of Indium Atoms in g‐C3N4 for Ameliorating Hydrogen Peroxide Piezo‐Photogeneration

Unraveling Precise Locations of Indium Atoms in g‐C3N4 for Ameliorating Hydrogen Peroxide Piezo‐Photogeneration

Insights into Molten Salts Induced Structural Defects in Graphitic Carbon Nitrides for Piezo‐Photocatalysis with Multiple H2O2 Production Channels

Unraveling Precise Locations of Indium Atoms in g-C3N4 for Ameliorating Hydrogen Peroxide Piezo-Photogeneration

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Product

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Unraveling Precise Locations of Indium Atoms in g‐C₃N₄ for Ameliorating Hydrogen Peroxide Piezo‐Photogeneration

Unraveling Precise Locations of Indium Atoms in g‐C₃N₄ for Ameliorating Hydrogen Peroxide Piezo‐Photogeneration

Insights into Molten Salts Induced Structural Defects in Graphitic Carbon Nitrides for Piezo‐Photocatalysis with Multiple H₂O₂ Production Channels