Insights into the role of C-S-C bond in C3N5 for photocatalytic NO deep oxidation: Experimental and DFT exploration

Zhang, Junlei; Li, Zhi; Liu, Bin; Chen, Mengshan; Zhou, Yingtang; Zhu, Mingshan

doi:10.1016/j.apcatb.2023.122522

Cited by 24 publications

(7 citation statements)

References 55 publications

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“…Finally, C 3 N 5 /Fe 2 O 3 photocatalysts were synthesized via the annealing treatment in the air (Figure S1). As suggested in Figure 1B 35 The C 1s (Figure 1G) has two peaks at 288.1 and 284.8 eV, which is caused by the sp 3 and sp 2 hybridized carbon. 36 The sp 3 peak is attributed to the adventitious carbon in C 3 N 5 polymers and the sp 2 is related to N = C-N aromatic carbon, thus building a basic skeleton for C 3 N 5 .…”

Section: Resultsmentioning

confidence: 83%

“…To demonstrate the strong electronic coupling in the C 3 N 5 /Fe 2 O 3 heterostructure, the chemical states of each element are investigated by HRXPS. As shown in Figure 1F, the N 1s characteristic signal is deconvolved into two peaks at binding energies of 398.6 and 400.2 eV, corresponding to the tertiary N –(C) 3 /secondary C = N–C and the residual –NH 2 /bridging C–N = N–C 35 . The C 1s (Figure 1G) has two peaks at 288.1 and 284.8 eV, which is caused by the sp 3 and sp 2 hybridized carbon 36 .…”

Section: Resultsmentioning

confidence: 99%

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Photo‐enhanced uranium recovery from spent fuel reprocessing wastewater via S‐scheme 2D/0D C₃N₅/Fe₂O₃ heterojunctions

Meng,

Wu,

Yang

et al. 2024

SusMat

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Re‐extracting environmentally transportable hexavalent uranium from wastewater produced by spent fuel reprocessing using the photocatalytic technology is a crucial strategy to avoid uranium pollution and recover nuclear fuel strategic resources. Here, we have designed S‐scheme 2D/0D C3N5/Fe2O3 heterojunction photocatalysts based on the built‐in electric field and the energy band bending theory, and have further revealed the immobilization process of hexavalent uranium conversion into relatively insoluble tetravalent uranium in terms of thermodynamics and kinetics. According to the results, the hexavalent uranium removal and recovery ratios in wastewater are as high as 93.38% and 83.58%, respectively. Besides, C3N5/Fe2O3 heterojunctions also exhibit satisfactory catalytic activity and selectivity even in the presence of excessive impurity cations (including Na+, K+, Ca2+, Mg2+, Sr2+, and Eu3+) or various organics (such as xylene, tributylphosphate, pyridine, tannic acid, citric acid, and oxalic acid). It is believed that this work can provide a potential opportunity for S‐scheme heterojunction photocatalysts to re‐enrich uranium from spent fuel wastewater.

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Section: Resultsmentioning

confidence: 83%

Section: Resultsmentioning

confidence: 99%

Photo‐enhanced uranium recovery from spent fuel reprocessing wastewater via S‐scheme 2D/0D C₃N₅/Fe₂O₃ heterojunctions

Meng,

Wu,

Yang

et al. 2024

SusMat

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“…Finally, Figure 3e exhibits the presence of S 2p in CN, S-VO x , and S-VOCN with different S species with the oxidation of +2 in the samples, including SO 3 2− and C−S−C. 48,49 As a result, the evidence from the XPS spectra validates the successful synthesis of the designed composites and the charge transportation in the dark to balance the Fermi level of the composites from CN to VO x or S-VO x , which would be related to S-scheme charge transfer mechanisms in the dark.…”

Section: Resultsmentioning

confidence: 98%

Simultaneously Utilizing Excited Holes and Electrons for Piezoelectric-Enhanced Photoproduction of H₂O₂ from S-Scheme 2D S-Doped VO_x/g-C₃N₄ Nanostructures

Phuoc Toan,

Nguyen,

Phan

et al. 2024

ACS Appl. Mater. Interfaces

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2D/2D step-scheme (S-scheme) piezo-photocatalysts for the production of fine chemicals, such as hydrogen peroxide (H2O2), have attracted significant attention of global scientists owing to the efficiency in utilizing surface piezoelectric effects from 2D materials to overcome rapid charge recombination in photocatalytic processes. In this research, we reported the fabrication of 2D S-doped VO x deposited on 2D g-C3N4 to produce H2O2 via the piezo-photocatalytic process with high production yields at 20.19 mmol g–1 h–1, which was 1.75 and 4.87 times higher than that from solely piezo-catalytic and photocatalytic H2O2 generation. The finding pointed out that adding sulfur (S) to VO x can help to improve the catalytic outcomes by modifying the electronic properties of pristine VO x . In addition, when coupled with g-C3N4, the presence of S limits the formation of graphene in the VO x /g-C3N4 composites, causing shielding effects and pushing the cascade reactions toward water generation in the materials. Besides, the research also sheds light on the charge transport between g-C3N4 and S-VO x under irradiation and how the composites work to trigger the formation of H2O2. The presence of S in the composite systems enhances charge transfer between two semiconductors by strengthening the internal electric fields (IEF) to drive electrons moving in one direction, as demonstrated by density functional theory (DFT) calculations. Moreover, the formation of H2O2 significantly relies on the reduction of oxygen to generate oxygenic radical species at the g-C3N4 sites. Meanwhile, S-VO x provides oxidative sites in the composites to oxidize water molecules to directly or indirectly generate H2O2 or O2, which will further participate in the reactions to produce the final products. This study confirms the validation of S-scheme piezo-photocatalysts, thus encouraging further research on developing heterojunction materials with high catalytic efficiency, which can be used in practical conditions.

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“…On the surface of a photocatalyst, photogenerated electrons and holes interact with adsorbed species such as O2 and H2O, leading to the formation of reactive oxygen species (ROS) with potent oxidizing properties [29]. These ROS, including superoxide (•O2 − ), peroxide (O2 2− ), and hydrogen peroxide (H2O2), are capable of reacting with nitrogen oxides (NO) to form nitrates and NO2 (Figure 2) [3,30].…”

Section: Photocatalytic No X Removal Mechanism and Chemistrymentioning

confidence: 99%

Section: Photocatalytic No X Removal Mechanism and Chemistrymentioning

confidence: 99%

Materials Design and Development of Photocatalytic NOx Removal Technology

Bari,

Islam,

Jeong

2024

Metals

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Nitrogen oxide (NOx) pollutants have a significant impact on both the environment and human health. Photocatalytic NOx removal offers a sustainable and eco-friendly approach to combatting these pollutants by harnessing renewable solar energy. Photocatalysis demonstrates remarkable efficiency in removing NOx at sub-scale levels of parts per billion (ppb). The effectiveness of these catalysts depends on various factors, including solar light utilization efficiency, charge separation performance, reactive species adsorption, and catalytic reaction pathway selectivity. Moreover, achieving high stability and efficient photocatalytic activity necessitates a multifaceted materials design strategy. This strategy encompasses techniques such as ion doping, defects engineering, morphology control, heterojunction construction, and metal decoration on metal- or metal oxide-based photocatalysts. To optimize photocatalytic processes, adjustments to band structures, optimization of surface physiochemical states, and implementation of built-in electric field approaches are imperative. By addressing these challenges, researchers aim to develop efficient and stable photocatalysts, thus contributing to the advancement of environmentally friendly NOx removal technologies. This review highlights recent advancements in photocatalytic NOx removal, with a focus on materials design strategies, intrinsic properties, fundamental developmental aspects, and performance validation. This review also presents research gaps, emphasizing the need to understand the comprehensive mechanistic photocatalytic process, favored conditions for generating desired reactive species, the role of water concentration, temperature effects, inhibiting strategies for photocatalyst-deactivating species, and the formation of toxic NO2.

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Insights into the role of C-S-C bond in C3N5 for photocatalytic NO deep oxidation: Experimental and DFT exploration

Cited by 24 publications

References 55 publications

Photo‐enhanced uranium recovery from spent fuel reprocessing wastewater via S‐scheme 2D/0D C₃N₅/Fe₂O₃ heterojunctions

Photo‐enhanced uranium recovery from spent fuel reprocessing wastewater via S‐scheme 2D/0D C₃N₅/Fe₂O₃ heterojunctions

Simultaneously Utilizing Excited Holes and Electrons for Piezoelectric-Enhanced Photoproduction of H₂O₂ from S-Scheme 2D S-Doped VO_x/g-C₃N₄ Nanostructures

Materials Design and Development of Photocatalytic NOx Removal Technology

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Insights into the role of C-S-C bond in C3N5 for photocatalytic NO deep oxidation: Experimental and DFT exploration

Cited by 24 publications

References 55 publications

Photo‐enhanced uranium recovery from spent fuel reprocessing wastewater via S‐scheme 2D/0D C3N5/Fe2O3 heterojunctions

Photo‐enhanced uranium recovery from spent fuel reprocessing wastewater via S‐scheme 2D/0D C3N5/Fe2O3 heterojunctions

Simultaneously Utilizing Excited Holes and Electrons for Piezoelectric-Enhanced Photoproduction of H2O2 from S-Scheme 2D S-Doped VOx/g-C3N4 Nanostructures

Materials Design and Development of Photocatalytic NOx Removal Technology

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Photo‐enhanced uranium recovery from spent fuel reprocessing wastewater via S‐scheme 2D/0D C₃N₅/Fe₂O₃ heterojunctions

Photo‐enhanced uranium recovery from spent fuel reprocessing wastewater via S‐scheme 2D/0D C₃N₅/Fe₂O₃ heterojunctions

Simultaneously Utilizing Excited Holes and Electrons for Piezoelectric-Enhanced Photoproduction of H₂O₂ from S-Scheme 2D S-Doped VO_x/g-C₃N₄ Nanostructures