Graphitic carbon nitride nanosheets with low O<sub>N1</sub>-doping content as efficient photocatalysts for organic pollutant degradation

Huang, Yan; Ning, Lichao; Feng, Zibo; Ma, Guifeng; Yang, Shuliang; Su, Yongxuan; Hong, Yanzhen; Wang, Hongtao; Li, Peng; Li, Jun

doi:10.1039/d0en01198c

Cited by 20 publications

(8 citation statements)

References 48 publications

(69 reference statements)

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“…More importantly, the electronic structure was optimized greatly, as reflected by the charge distribution map of H 2 ‐O 2 ‐pCN, which obviously provided local asymmetric electron environment to promote the migration of electrons, thus served as H 2 evolution active center. [ 41–43 ] This local asymmetric electronic structure is also conducive to the adsorption of hydrogen ions and further promotes the production of H 2 . In general, the construction of carboxyl deficient carbon nitride is an important idea to improve the performance of photocatalytic hydrogen production.…”

Section: Resultsmentioning

confidence: 99%

Unraveling Structural Carboxyl Defects in g‐C₃N₄ for Improved Photocatalytic H₂ Evolution via Alternating Hydrogen‐Oxygen‐Plasma Treatment

Chang

Wang

et al. 2022

Advanced Sustainable Systems

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Structural defect‐endowed photocatalysts are being increasingly recognized due to the enhanced catalytic activity of multiple defect sites (e.g., vacancies or functional groups). However, because of the excessive destruction effect of conventional chemical oxidation methods toward carboxyl defects engineering, the mechanism is still unclear and practice is rare in developing high‐quality structural carboxyl defect‐involved g‐C3N4. Herein, an alternating hydrogen‐oxygen‐plasma treatment is proposed to endow the g‐C3N4 with enriched vacancy defect sites for the subsequent immobilization of carboxyl groups, thus overcoming the problem of lacking of covalent binding sites in g‐C3N4 in developing carboxyl defective g‐C3N4 photocatalysts. The alternating hydrogen‐oxygen‐plasma treatment does not only influence the defect structure of g‐C3N4, but also changes its morphology, optimizes the electronic distribution, and increases the separation efficiency of photogenerated electrons and holes, thereby increasing photocatalytic H2 evolution by 7.91 times. Density functional calculations and electrochemical characterization suggest that the carboxyl defects generated by the fast H2‐O2 plasma modification lead to a local asymmetric electron environment, which enhances carrier separation capability and significantly improves H2 generation activity. This study provides a new insight into the rational design and fabrication of defect‐containing photocatalysts, carbon materials, and polymers.

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Section: Resultsmentioning

confidence: 99%

Unraveling Structural Carboxyl Defects in g‐C₃N₄ for Improved Photocatalytic H₂ Evolution via Alternating Hydrogen‐Oxygen‐Plasma Treatment

Chang

Wang

et al. 2022

Advanced Sustainable Systems

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“…The C 1s spectrum of bulk g-C 3 N 4 exhibited three peaks at 284.8, 285.6, 288, and 289 eV which correspond to C–C or CC bonds, the combination of C–N groups, C–NC of the tri- s -triazine network, and superficial C–O species, respectively . The N 1s spectrum of bulk g-C 3 N 4 exhibited three different nitrogen species at 398.5 and 400.5, which are assigned to the C–NC of the tri- s -triazine network and [C] 3 –N, respectively. The O 1s spectrum of bulk g-C 3 N 4 showed a peak at 532.6 eV of the O atom bonded to sp 2 -hybridized carbon .…”

Section: Resultsmentioning

confidence: 99%

Photocatalytic Partial Oxidation of 5-Hydroxymethylfurfural to 2,5-Diformylfuran Using Exfoliated g-C₃N₄/Pd Nanoarchitectures

et al. 2022

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Graphitic carbon nitride (g-C 3 N 4 ) can trigger the photocatalytic partial oxidation of HMF to produce 2,5-diformylfuran (DFF), yet limitations still exist in improving its performance. Herein, Pd nanoparticles were deposited over thermally exfoliated g-C 3 N 4 (Ex-g-C 3 N 4 ) to boost its activity. Graphitic sheets with a thickness of ∼1.2−1.6 nm were obtained and then decorated with spherical Pd nanoparticles with a size of 2.0−2.5 nm. A maximum concentration of DFF (148.5 ± 4.9 μM) was obtained over the Ex-g-C 3 N 4 /Pd with 6% (w/w) deposited Pd with a product selectivity toward DFF of 42.9 ± 0.6%. Our results revealed that the extent of DFF production is directly proportional to the Pd content until 6% (w/w), and beyond that it declines. Trapping experiments and EPR analysis showed that singlet oxygen is the dominant species responsible for the selective oxidation of HMF to DFF. Our mechanistic study suggests that triplet excitons are generated via intersystem crossing, which then react with molecular oxygen to produce singlet oxygen. Furthermore, intrinsic reaction coordinate and energy barrier calculations indicated that the reaction is thermodynamically allowable. Our study reveals that singlet oxygen is capable of abstracting hydrogen atoms from the α carbon and hydroxyl moiety of HMF to eventually produce DFF. This work provides deep insight into the benefits of exploiting Pd nanoparticles to enhance production of singlet oxygen over g-C 3 N 4 , which in turn enhances the production of DFF.

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“…The photogenerated electron-hole pairs can be used directly and effectively, thereby improving the photocatalytic efficiency. If the dye has a weak polarity and is easy to disperse in the solution, some electrons will be annihilated [73].…”

Section: Photocatalytic Degradation Performancesmentioning

confidence: 99%

Carbene Ligand-Doped Fe2O3 Composite for Rapid Removal of Multiple Dyes under Sunlight

et al. 2021

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Contaminated water due to industrial organic dyes presents a significant challenge to sustainability. As a material of green energy, photocatalysts offer an effective and environmentally friendly way to deal with organic dyes for water treatment. A series of simple and highly efficient iron photocatalysts with carbene ligands were developed, which, under the illumination of sunlight, can rapidly degrade multiple organic dyes in water at room temperature, including rhodamine B (RhB), indigo carmine (IC), methyl blue (MB), and congo red (CR). The field-only surface integral method was carried out to determine the absorption spectrum of photocatalyst particles. Under the optimized experimental conditions which were selected by the orthogonal experiments for four dyes, 0.5a@Fe2O3 and 2c@Fe2O3 demonstrated good stability and photocatalytic activity. These two composite materials not only have the ability to remove 98.0% of the degradation in 10 s, but also maintain high reactivity after a few cycles of repeated use.

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Graphitic carbon nitride nanosheets with low O_N1-doping content as efficient photocatalysts for organic pollutant degradation

Abstract: ON1-Doped g-C3N4 nanosheets with low oxygen content showed a greatly enhanced photocatalytic performance for the degradation of organic pollutants.

Cited by 20 publications

References 48 publications

Unraveling Structural Carboxyl Defects in g‐C₃N₄ for Improved Photocatalytic H₂ Evolution via Alternating Hydrogen‐Oxygen‐Plasma Treatment

Unraveling Structural Carboxyl Defects in g‐C₃N₄ for Improved Photocatalytic H₂ Evolution via Alternating Hydrogen‐Oxygen‐Plasma Treatment

Photocatalytic Partial Oxidation of 5-Hydroxymethylfurfural to 2,5-Diformylfuran Using Exfoliated g-C₃N₄/Pd Nanoarchitectures

Carbene Ligand-Doped Fe2O3 Composite for Rapid Removal of Multiple Dyes under Sunlight

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Graphitic carbon nitride nanosheets with low ON1-doping content as efficient photocatalysts for organic pollutant degradation

Abstract: ON1-Doped g-C3N4 nanosheets with low oxygen content showed a greatly enhanced photocatalytic performance for the degradation of organic pollutants.

Cited by 20 publications

References 48 publications

Unraveling Structural Carboxyl Defects in g‐C3N4 for Improved Photocatalytic H2 Evolution via Alternating Hydrogen‐Oxygen‐Plasma Treatment

Unraveling Structural Carboxyl Defects in g‐C3N4 for Improved Photocatalytic H2 Evolution via Alternating Hydrogen‐Oxygen‐Plasma Treatment

Photocatalytic Partial Oxidation of 5-Hydroxymethylfurfural to 2,5-Diformylfuran Using Exfoliated g-C3N4/Pd Nanoarchitectures

Carbene Ligand-Doped Fe2O3 Composite for Rapid Removal of Multiple Dyes under Sunlight

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Graphitic carbon nitride nanosheets with low O_N1-doping content as efficient photocatalysts for organic pollutant degradation

Unraveling Structural Carboxyl Defects in g‐C₃N₄ for Improved Photocatalytic H₂ Evolution via Alternating Hydrogen‐Oxygen‐Plasma Treatment

Unraveling Structural Carboxyl Defects in g‐C₃N₄ for Improved Photocatalytic H₂ Evolution via Alternating Hydrogen‐Oxygen‐Plasma Treatment

Photocatalytic Partial Oxidation of 5-Hydroxymethylfurfural to 2,5-Diformylfuran Using Exfoliated g-C₃N₄/Pd Nanoarchitectures