Heterogeneous structural defects to prompt charge shuttle in g-C3N4 plane for boosting visible-light photocatalytic activity

Yang, Chengwu; Xue, Zhe; Qin, Jiaqian; Sawangphruk, Montree; Zhang, Xinyu; Liu, Riping

doi:10.1016/j.apcatb.2019.118094

Cited by 108 publications

(45 citation statements)

References 37 publications

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“…However, further detection indicates that the CCN samples exhibit an additional peak at 2180 cm −1 , matching with the asymmetric stretching vibration of CN (cyano‐groups). [ 50 ] Moreover, with increasing Na 2 CO 3 dosage, a gradually enhanced cyano‐group peak can be significantly detected, suggesting the generation of cyano‐groups (CN) on the resultant crystalline g‐C 3 N 4 surface.…”

Section: Resultsmentioning

confidence: 99%

One‐Step Realization of Crystallization and Cyano‐Group Generation for g‐C₃N₄ Photocatalysts with Improved H₂ Production

et al. 2020

Solar RRL

104

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In contrast to conventional disordered g‐C3N4, the ordered arrangement of s‐triazine units and cyano‐group is important for its improved photocatalytic H2 evolution activity. However, the usual synthetic methods include complex, multiple‐step operations or containing the use of toxic materials. Herein, the ordered crystallization and cyano‐group generation are simultaneously realized for the g‐C3N4 photocatalyst (namely, cyano‐group‐modified crystalline g‐C3N4) by a facile and green one‐step Na2CO3‐assisted synthesis approach. It is found that Na2CO3 first effectively promotes the denitrification of dicyandiamide (DCDA) and accelerates its polymerization to produce highly crystalline g‐C3N4. When the temperature is over 500 °C, Na2CO3 facilitates the pyrolysis of partial s‐triazine units to produce cyano‐groups on the g‐C3N4 surface, resulting in the final generation of cyano‐group‐modified crystalline g‐C3N4. Consequently, the resulting cyano‐group‐modified crystalline g‐C3N4 presents a highly increased hydrogen production activity, about twofold higher than that of the bulk g‐C3N4. The increased hydrogen production activity is primarily because of the synergistic effect of the highly crystalline and cyano‐group functional for the resulting cyano‐group‐modified crystalline g‐C3N4. The current technology opens insights for the preparation of other crystalline photocatalysts.

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Section: Resultsmentioning

confidence: 99%

One‐Step Realization of Crystallization and Cyano‐Group Generation for g‐C₃N₄ Photocatalysts with Improved H₂ Production

et al. 2020

Solar RRL

104

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“…The peaks located at 13.13°and 27.5°are consistent with the (100) plane of in-plane structural packing and the (002) plane of the interlayer stacking of conjugated aromatic segments of g-C 3 N 4 , respectively. [13] Compared with the g-C 3 N 4 , the above two characteristic diffraction peaks of pg-C 3 N 4 show the weaker intensity caused by the pore defects, as well as those of Au/pg-C 3 N 4 . With the increase of loading amounts of Au nanoparticles, four peaks at 38.2°, 44.4°, 64.6°, and 77.5°corresponding to (111), (200), (220), and (311) planes of Au nanoparticles, respectively, [26] have the gradually increased intensity.…”

Section: Xrdmentioning

confidence: 93%

“…[9][10][11] However, g-C 3 N 4 prepared by traditional thermal polymerization method has the disadvantages of low specific surface area, low visiblelight utilization, and high recombination rate of photogenerated electrons and holes, resulting to a low photocatalytic activity. [12] Aiming at above issues, a variety of strategies to enhance the photocatalytic activity of g-C 3 N 4 have been proposed, such as structural modification, [13,14] elemental doping, [15,16] and heterojunction construction by combining other semiconductors and nanostructures. [17,18] Plasmonic metallic nanoparticles, such as Au, Ag and Pt, can enhance light absorption by the localized surface plasmon resonance (LSPR) effect and transfer the electrons as the carrier to promote photogenerated electron-hole separation.…”

Section: Introductionmentioning

confidence: 99%

Photocatalytic Degradation of Organic Pollutants Using Porous g‐C₃N₄ Nanosheets Decorated with Gold Nanoparticles

Cong

Wang

et al. 2021

ChemistrySelect

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In this work, a composite photocatalyst consisted of the porous graphitic carbon nitride (pg-C 3 N 4 ) nanosheets decorated with in-situ grown gold (Au) nanoparticles were prepared. By characterizing and analyzing chemical compositions and structures, and optical and electrical properties of this Au/pg-C 3 N 4 composite, the excellent photocatalytic performance mainly comes from the following aspects: firstly, pg-C 3 N 4 synthesized from melamine by high-temperature calcination with the assistance of ascorbic acid has larger specific surface area and narrower band gap width than common g-C 3 N 4 ; secondly, localized surface plasmon resonance (LSPR) effect of Au nanoparticles can enhance light absorption of pg-C 3 N 4 via near-field enhancement-induced excitation; thirdly, the heterojunction formed between Au nanoparticles and pg-C 3 N 4 nanosheets can promote electron transfer. Consequently, Au/pg-C 3 N 4 presented the obvious improvement of photocatalytic activity on the degradation of rhodamine B and amaranth under simulated solar irradiation that the kinetic rate constant of degradation reaction can be increased by 3.9 and 5.7 times compared with g-C 3 N 4 , respectively.

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“…This implies that spatial separation occurs on the surface of the N‐defect mediated g‐C 3 N 4 . Meanwhile, the shuttling channel formed on the bridge nitrogen atoms lends itself to fast electron transfer across the heptazine rings 113 . In terms of the roles of N‐vacancies on band gap tuning, the Fermi level was raised to the bottom of the CB to induce a metallic property in the modified carbon nitride, 114 as well as a reduced band gap and a red‐shifted optical absorption, resulting in an increase in low‐energy photon excitation 115,116 .…”

Section: Role Of Carbon Nitride Modification Strategiesmentioning

confidence: 99%

Solar‐powered chemistry: Engineering low‐dimensional carbon nitride‐based nanostructures for selective CO₂ conversion to C₁C₂ products

Foo

Ong

2022

InfoMat

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CO2 capture and conversion has been prospected as an auspicious technology to simultaneously tackle the rise in global CO2 emission and produce value‐added fuels with the goal of accomplishing carbon neutrality. A sustainable route to achieve this is via the utilization of solar energy, thereby harnessing the abundant and nonexhaustive resource to shift our reliance away from rapidly depleting fossil fuels. Graphitic carbon nitride (g‐C3N4) and its allotrope have earned its rank as a fascinating metal‐free photocatalyst due to its superior stability, high surface‐area‐to‐volume ratio, and tunable surface engineering. By leveraging these properties, robust carbon nitride‐based nanostructures are engineered for photocatalytic CO2 conversion to energy‐rich C1C2 product, which is indispensable in the chemical industry. Thus, this review presents the latest panorama of experimental and computational research on tuning the local electronic, surface chemical coordination environment, charge dynamics and optical properties of low‐dimensional carbon nitride and its allotropes toward highly selective and efficient CO2 photoconversion. To name a few, structural engineering, point‐defect engineering, heterojunction construction, and cocatalyst loading. To advance this frontier, critical insights are elucidated to establish the structure‐performance relationship and unravel primary factors dictating the selectivity of C1C2 molecules from CO2 reduction. External‐field assisted photocatalysis such as with electric (photoelectro‐) and heat (photothermal) is discussed to uncover the synergistic contributions that drive the development in photochemistry. Last, future challenges and prospects are outlined for the potential application of solar‐driven CO2 conversion, along with the scale‐up strategy from the economic viewpoint toward the rational development of high‐efficiency carbon nitride catalysts.

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Heterogeneous structural defects to prompt charge shuttle in g-C3N4 plane for boosting visible-light photocatalytic activity

Cited by 108 publications

References 37 publications

One‐Step Realization of Crystallization and Cyano‐Group Generation for g‐C₃N₄ Photocatalysts with Improved H₂ Production

One‐Step Realization of Crystallization and Cyano‐Group Generation for g‐C₃N₄ Photocatalysts with Improved H₂ Production

Photocatalytic Degradation of Organic Pollutants Using Porous g‐C₃N₄ Nanosheets Decorated with Gold Nanoparticles

Solar‐powered chemistry: Engineering low‐dimensional carbon nitride‐based nanostructures for selective CO₂ conversion to C₁C₂ products

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Heterogeneous structural defects to prompt charge shuttle in g-C3N4 plane for boosting visible-light photocatalytic activity

Cited by 108 publications

References 37 publications

One‐Step Realization of Crystallization and Cyano‐Group Generation for g‐C3N4 Photocatalysts with Improved H2 Production

One‐Step Realization of Crystallization and Cyano‐Group Generation for g‐C3N4 Photocatalysts with Improved H2 Production

Photocatalytic Degradation of Organic Pollutants Using Porous g‐C3N4 Nanosheets Decorated with Gold Nanoparticles

Solar‐powered chemistry: Engineering low‐dimensional carbon nitride‐based nanostructures for selective CO2 conversion to C1C2 products

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Product

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One‐Step Realization of Crystallization and Cyano‐Group Generation for g‐C₃N₄ Photocatalysts with Improved H₂ Production

One‐Step Realization of Crystallization and Cyano‐Group Generation for g‐C₃N₄ Photocatalysts with Improved H₂ Production

Photocatalytic Degradation of Organic Pollutants Using Porous g‐C₃N₄ Nanosheets Decorated with Gold Nanoparticles

Solar‐powered chemistry: Engineering low‐dimensional carbon nitride‐based nanostructures for selective CO₂ conversion to C₁C₂ products