Polyhedral oligomeric silsesquioxane as a recyclable soft template to synthesize mesoporous polymeric carbon nitride with enhanced photocatalytic hydrogen evolution

Liang, Zhiwei; Liu, Lei; Zhuang, Xiaojia; Tang, Zicheng; Li, Haiping; Kang, Wenbing

doi:10.1039/d0se01388a

Cited by 6 publications

(2 citation statements)

References 38 publications

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“…In recent years, two-dimensional (2D) ultrathin g-C 3 N 4 nanosheets with porous structures have drawn much interest due to their tunable electronic structure, high specific surface area, and short charge migration length . So far, various morphologies such as nanosheets, nanotubes, porous structures, and three-dimensional structures have been successfully synthesized through several typical methods, such as hard templating, soft templating, , self-templating, , and ultrasonic exfoliation methods . Among them, self-templating strategies (e.g., supramolecular self-assembly) have received much attention in the formation of hydrogen-bonded supramolecular compounds between melamine precursors and triazine derivatives.…”

Section: Introductionmentioning

confidence: 99%

Interlayer Potassium Single-Atom-Coordinated g-C₃N₄ for Significantly Boosted Visible Light Photocatalytic H₂ Production

Lu,

Yuan,

Chen

et al. 2024

Langmuir

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In recent years, graphitic carbon nitride (g-C3N4) has attracted considerable attention because it includes earth-abundant carbon and nitrogen elements and exhibits good chemical and thermal stability owing to the strong covalent interaction in its conjugated layer structure. However, bulk g-C3N4 has some disadvantages of low specific surface area, poor light absorption, rapid recombination of photogenerated charge carriers, and insufficient active sites, which hinder its practical applications. In this study, we design and synthesize potassium single-atom (K SAs)-doped g-C3N4 porous nanosheets (CM-KX, where X represents the mass of KHP added) via supramolecular self-assembling and chemical cross-linking copolymerization strategies. The results show that the utilization of supramolecules as precursors can produce g-C3N4 nanosheets with reduced thickness, increased surface area, and abundant mesopores. In addition, the intercalation of K atoms within the g-C3N4 nitrogen pots through the formation of K–N bonds results in the reduction of the band gap and expansion of the visible-light absorption range. The optimized K-doped CM-K12 nanosheets achieve a specific surface area of 127 m2 g–1, which is 11.4 times larger than that of the pristine g-C3N4 nanosheets. Furthermore, the optimal CM-K12 sample exhibits the maximum H2 production rate of 127.78 μmol h–1 under visible light (λ ≥ 420 nm), which is nearly 23 times higher than that of bare g-C3N4. This significant improvement of photocatalytic activity is attributed to the synergistic effects of the mesoporous structure and K SAs doping, which effectively increase the specific surface area, improve the visible-light absorption capacity, and facilitate the separation and transfer of photogenerated electron–hole pairs. Besides, the optimal sample shows good chemical stability for 20 h in the recycling experiments. Density functional theory calculations confirm that the introduction of K SAs significantly boosts the adsorption energy for water and decreases the activation energy barrier for the reduction of water to hydrogen.

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Section: Introductionmentioning

confidence: 99%

Interlayer Potassium Single-Atom-Coordinated g-C₃N₄ for Significantly Boosted Visible Light Photocatalytic H₂ Production

Lu,

Yuan,

Chen

et al. 2024

Langmuir

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“…Pore modification methods of g -C 3 N 4 can be generally categorized into three types: hard-template method [ 51 , 52 , 53 , 54 ], soft-template method [ 55 , 56 , 57 , 58 , 59 ], and template-free method [ 60 , 61 , 62 , 63 ] ( Figure 2 ). Hard template provides good support in yielding relatively regular pores that can act as a good channel for the migration of photogenerated charge.…”

Section: Introductionmentioning

confidence: 99%

g-C3N4: Properties, Pore Modifications, and Photocatalytic Applications

et al. 2021

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Graphitic carbon nitride (g-C3N4), as a polymeric semiconductor, is promising for ecological and economical photocatalytic applications because of its suitable electronic structures, together with the low cost, facile preparation, and metal-free feature. By modifying porous g-C3N4, its photoelectric behaviors could be facilitated with transport channels for photogenerated carriers, reactive substances, and abundant active sites for redox reactions, thus further improving photocatalytic performance. There are three types of methods to modify the pore structure of g-C3N4: hard-template method, soft-template method, and template-free method. Among them, the hard-template method may produce uniform and tunable pores, but requires toxic and environmentally hazardous chemicals to remove the template. In comparison, the soft templates could be removed at high temperatures during the preparation process without any additional steps. However, the soft-template method cannot strictly control the size and morphology of the pores, so prepared samples are not as orderly as the hard-template method. The template-free method does not involve any template, and the pore structure can be formed by designing precursors and exfoliation from bulk g-C3N4 (BCN). Without template support, there was no significant improvement in specific surface area (SSA). In this review, we first demonstrate the impact of pore structure on photoelectric performance. We then discuss pore modification methods, emphasizing comparison of their advantages and disadvantages. Each method’s changing trend and development direction is also summarized in combination with the commonly used functional modification methods. Furthermore, we introduce the application prospects of porous g-C3N4 in the subsequent studies. Overall, porous g-C3N4 as an excellent photocatalyst has a huge development space in photocatalysis in the future.

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Mesoporous Carbon Nitrides as Emerging Materials: Nanoarchitectonics and Biosensing Applications

Patel¹,

Baskar²,

Tiburcius³

et al. 2023

Advanced Sensor Research

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Mesoporous carbon nitrides (MCNs) are versatile materials and find use in applications such as catalysis, gas capture, and remediation. The development of new forms of MCNs, such as C3N5, C3N6, and C3N7, has expanded their scope further. One of the least reviewed applications of these materials is in the field of sensing, though it has been demonstrated that their sensing abilities are on par with other comparable materials. Their excellent properties such as high surface area, tunable stoichiometry, adjustable electronic structure, and basicity, make them well‐suited for the adsorption and detection of a wide range of analytes. Herein, the new findings in the synthesis of MCNs and their exciting prospects for sensing are reviewed. The review is divided into two broad sections: 1) discussions on the synthesis of MCNs using hard/soft templating, sol–gel, and template‐free methods; and 2) their capabilities for photoelectrochemical, optical, and quartz microbalance‐based sensing. The findings from the recent literature are showcased and the covered topics are explained with comparative analyses. The current review is a timely presentation of the concerned topic and will serve as a useful piece of information for developing advanced sensors using MCN based materials.

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Polyhedral oligomeric silsesquioxane as a recyclable soft template to synthesize mesoporous polymeric carbon nitride with enhanced photocatalytic hydrogen evolution

Abstract: A novel recyclable template was used to prepare mesoporous polymeric carbon nitride with prominently increased specific surface area and photoactivity.

Cited by 6 publications

References 38 publications

Interlayer Potassium Single-Atom-Coordinated g-C₃N₄ for Significantly Boosted Visible Light Photocatalytic H₂ Production

Interlayer Potassium Single-Atom-Coordinated g-C₃N₄ for Significantly Boosted Visible Light Photocatalytic H₂ Production

g-C3N4: Properties, Pore Modifications, and Photocatalytic Applications

Mesoporous Carbon Nitrides as Emerging Materials: Nanoarchitectonics and Biosensing Applications

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Polyhedral oligomeric silsesquioxane as a recyclable soft template to synthesize mesoporous polymeric carbon nitride with enhanced photocatalytic hydrogen evolution

Abstract: A novel recyclable template was used to prepare mesoporous polymeric carbon nitride with prominently increased specific surface area and photoactivity.

Cited by 6 publications

References 38 publications

Interlayer Potassium Single-Atom-Coordinated g-C3N4 for Significantly Boosted Visible Light Photocatalytic H2 Production

Interlayer Potassium Single-Atom-Coordinated g-C3N4 for Significantly Boosted Visible Light Photocatalytic H2 Production

g-C3N4: Properties, Pore Modifications, and Photocatalytic Applications

Mesoporous Carbon Nitrides as Emerging Materials: Nanoarchitectonics and Biosensing Applications

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Product

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Interlayer Potassium Single-Atom-Coordinated g-C₃N₄ for Significantly Boosted Visible Light Photocatalytic H₂ Production

Interlayer Potassium Single-Atom-Coordinated g-C₃N₄ for Significantly Boosted Visible Light Photocatalytic H₂ Production