Construction of Graphitic C<sub>3</sub>N<sub>4</sub>-Based Intramolecular Donor–Acceptor Conjugated Copolymers for Photocatalytic Hydrogen Evolution

Fan, Xinghua; Zhang, Lingxia; Cheng, Ruolin; Wang, Min; Li, Mengli; Zhou, Yajun; Shi, Jianlin

doi:10.1021/acscatal.5b01155

Cited by 310 publications

(159 citation statements)

References 77 publications

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“…The hydrogen evolution rate was found to be strongly dependent on the linkage geometry of benzene unit in the polymer network and continuously increased from PrCMP‐1 to PrCMP‐3, and a maximum of 2.5 µmol h −1 was achieved for PrCMP‐3 without the cocatalyst of Pt. However, the hydrogen production rate of PrCMP‐3 increased to 12.1 µmol h −1 when 3 wt% Pt was added as cocatalyst (Figure c), which is almost five times higher than that of the bare PrCMP‐3 since the modification of Pt facilitates electron localization from the conduction band of the polymer to the deposited Pt nanoparticles and promotes hydrogen production . Similar results were also observed for PrCMP‐1 and PrCMP‐2 (Figure c).…”

Section: Resultssupporting

confidence: 68%

Perylene‐Containing Conjugated Microporous Polymers for Photocatalytic Hydrogen Evolution

Mao

Shi

et al. 2017

Macro Chemistry & Physics

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Three perylene‐containing conjugated microporous polymers (PrCMPs) are synthesized via Suzuki–Miyaura cross‐coupling reaction from perylene with four polymerizable functional groups and a range of different substituted benzene derivatives. The pore property and bandgap of the resulting PrCMPs can be tuned by changing the comonomer of benzene with different substituted groups and positions. The photocatalytic performances of the polymers are highly dependent on the surface area, geometry, and bandgap of the PrCMPs. It was found that the 1,2,4,5‐linked polymer of PrCMP‐3 shows the highest hydrogen evolution rate (HER) of 12.1 µmol h−1 under UV–vis light irradiation among the three polymers because of its high surface area, broad light absorption, and suitable bandgap. PrCMP‐3 also exhibits good photocatalytic stability for prolonged hydrogen production reaction. This result demonstrates that the crucial role of the linkage geometry offers a general principle for the rational design of conjugated microporous polymer photocatalysts.

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Section: Resultssupporting

confidence: 68%

Perylene‐Containing Conjugated Microporous Polymers for Photocatalytic Hydrogen Evolution

Mao

Shi

et al. 2017

Macro Chemistry & Physics

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“…[13,14] After the potential of g-C 3 N 4 was first observed, while focusing on the hydrogen evolution half-reaction, interest has begun to shift to achieving overall water splitting using these materials. [15,16] However, the exact structure of most g-C 3 N 4 materials is unknown and the synthesis usually involves high temperature processing, which offers limited scope for fine-tuning structure and properties.…”

mentioning

confidence: 99%

A Solution‐Processable Polymer Photocatalyst for Hydrogen Evolution from Water

Woods

Sprick

Smith

et al. 2017

Advanced Energy Materials

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exhibit photocatalytic hydrogen evolution in 2009, [12] and many advances have been made since then. [13,14] After the potential of g-C 3 N 4 was first observed, while focusing on the hydrogen evolution half-reaction, interest has begun to shift to achieving overall water splitting using these materials. [15,16] However, the exact structure of most g-C 3 N 4 materials is unknown and the synthesis usually involves high temperature processing, which offers limited scope for fine-tuning structure and properties. Also, while g-C 3 N 4 can be produced from inexpensive starting materials, the synthetic yield of the material is typically low. [15,17] Of special relevance here, graphitic carbon nitrides are insoluble solids: as for many inorganic catalysts, this can present challenges in terms of processing.Rather few organic photocatalysts have been studied for hydrogen evolution other than g-C 3 N 4 . Recently, nitrogencontaining poly(azomethine) networks and covalent triazinebased frameworks (CTFs) were shown to have photocatalytic activity with the addition of platinum cocatalysts. [18,19] We have shown that a series of conjugated microporous polymers (CMPs) could facilitate hydrogen evolution from water in the presence of a sacrificial electron donor, without any additional heavy metal cocatalyst. [20,21] Other CMPs have since been studied for photocatalysis [22,23] and recent studies have demonstrated that linear conjugated polymers can have high photocatalytic activities. [24,25] However, as with g-C 3 N 4 , none of these organic materials are soluble in common organic solvents. This insolu bility makes it more challenging to process these materials into functional composites. Moreover, photocatalysts are typically kept in suspension by stirring to prevent sedimentation, which results in loss of photocatalytic activity. [26] The loss of activity of insoluble catalysts can be prevented with the use of support substrates, [27] however, using solution processability allows the use of simpler supports and easier development of photoelectrodes.Soluble oligo(phenylene)s have been previously reported as photocatalysts, however, they displayed low activity, were only active under UV light, required a Ru cocatalyst and were only poorly soluble in organic solvents limiting processability. [28] More recently soluble metal-chelating polymers have been prepared although the photocatalytic activity of these polymers also appear to be very low with apparent quantum yields (AQY) below 3 × 10 −4 %. [29] The solubility of some alkylated conjugated polymers has also facilitated the preparation of polymer nanoparticles (PDots). [30,31] The preparation of these PDots enabled significant enhancements in rate over the pristine polymer although scalability and long-term stability of this approach has yet to be shown. Direct photocatalytic water splitting is an attractive strategy for clean energy production, but multicomponent nanostructured systems that mimic natural photosynthesis can be difficult to fabricate because of the insolubil...

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“…13,17 However, the practical applications of g-C 3 N 4 are still hindered by the several obstacles and shortcomings, especially its low specic surface area, limited active sites, poor adsorption ability, and the serious aggregation observed during a photocatalytic process, of common bulk g-C 3 N 4 prepared via the direct polycondensation of nitrogenrich precursors. 17,18 To overcome these drawbacks, many attempts, such as doping with heteroatoms, 19,20 constructing heterostructures, 21,22 fabricating copolymers, 23,24 and thermal etching, 25,26 have been dedicated towards improving the photocatalytic capability of g-C 3 N 4 . However, preparation of a highly active g-C 3 N 4 material using a facile and eco-friendly strategy is still desirable.…”

Section: Introductionmentioning

confidence: 99%

Highly efficient pollutant removal of graphitic carbon nitride by the synergistic effect of adsorption and photocatalytic degradation

et al. 2018

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Environmental remediation based on semiconducting materials offers a green solution for pollution control in water. Herein, we report a novel graphitic carbon nitride (g-C 3 N 4 ) by one-step polycondensation of urea.The novel g-C 3 N 4 material with a surface area of 114 m 2 g À1 allowed the repetitive adsorption of the rhodamine B (RhB) dye and facilitated its complete photocatalytic degradation upon light irradiation in 20 min. This study provides new insights into the fabrication of g-C 3 N 4 -based materials and facilitates their potential application in the synergistic removal of harmful organic pollutants in the field of water purification.

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Construction of Graphitic C₃N₄-Based Intramolecular Donor–Acceptor Conjugated Copolymers for Photocatalytic Hydrogen Evolution

Cited by 310 publications

References 77 publications

Perylene‐Containing Conjugated Microporous Polymers for Photocatalytic Hydrogen Evolution

Perylene‐Containing Conjugated Microporous Polymers for Photocatalytic Hydrogen Evolution

A Solution‐Processable Polymer Photocatalyst for Hydrogen Evolution from Water

Highly efficient pollutant removal of graphitic carbon nitride by the synergistic effect of adsorption and photocatalytic degradation

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Construction of Graphitic C3N4-Based Intramolecular Donor–Acceptor Conjugated Copolymers for Photocatalytic Hydrogen Evolution

Cited by 310 publications

References 77 publications

Perylene‐Containing Conjugated Microporous Polymers for Photocatalytic Hydrogen Evolution

Perylene‐Containing Conjugated Microporous Polymers for Photocatalytic Hydrogen Evolution

A Solution‐Processable Polymer Photocatalyst for Hydrogen Evolution from Water

Highly efficient pollutant removal of graphitic carbon nitride by the synergistic effect of adsorption and photocatalytic degradation

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Construction of Graphitic C₃N₄-Based Intramolecular Donor–Acceptor Conjugated Copolymers for Photocatalytic Hydrogen Evolution