Citation: Fangxin Yin, Pinquan Qin, Jingsan Xu, Shaowen Cao. Methylene Blue Incorporated Donor-Acceptor g-C3N4 Nanosheet Photocatalyst for H2 Production[J]. Acta Physico-Chimica Sinica, ;2023, 39(11): 221206. doi: 10.3866/PKU.WHXB202212062 shu

Methylene Blue Incorporated Donor-Acceptor g-C3N4 Nanosheet Photocatalyst for H2 Production

  • Corresponding author: Pinquan Qin, qinpqcu@whut.edu.cn Shaowen Cao, swcao@whut.edu.cn
  • Received Date: 31 December 2022
    Revised Date: 25 February 2023
    Accepted Date: 27 February 2023
    Available Online: 9 March 2023

    Fund Project: the National Key R & D Program of China 2022YFE0114800the National Natural Science Foundation of China 51922081

  • Photocatalytic hydrogen production is a promising strategy for utilizing inexhaustible solar energy as a source of clean energy. Graphitic carbon nitride (g-C3N4) is a widely used photocatalytic material in photocatalytic hydrogen production because of its simple preparation process, suitable band structure, and high stability. However, the low charge carrier separation efficiency and small specific surface area of pristine g-C3N4 restrict its photocatalytic activity. It has been demonstrated that the construction of intramolecular donor-acceptor (D-A) systems and ultra-thin nanosheet structures are effective strategies for enhancing the photocatalytic activity of g-C3N4. Herein, an intramolecular D-A structured g-C3N4 nanosheet photocatalyst is synthesized through the thermal copolymerization of dicyandiamide and methylene blue (MB), followed by thermal exfoliation. X-ray diffraction, Fourier transform infrared spectrometry, solid-state 13C nuclear magnetic resonance, and X-ray photoelectron spectroscopy analyses reveal that MB is successfully incorporated into the g-C3N4 framework and well retained after thermal exfoliation. The resulting D-A system induces intramolecular charge transfer from the donor units (MB segment) to the acceptor units (tri-s-triazine rings) and extends the absorption edge to approximately 500 nm. The ultra-thin nanosheet structure produced by thermal exfoliation shortens the charge transfer distance from the interior to the surface of g-C3N4 and reduces the charge transfer resistance, which increases the charge carrier separation efficiency. Furthermore, the introduction of MB generates a flaky structure during copolymerization, which promotes thermal exfoliation and results in a remarkably increased specific surface area. The transient photocurrent response, electrochemical impedance spectra, and time-resolved photoluminescence decay spectra reveal that the charge transfer and separation of g-C3N4 are further promoted by integrating the intramolecular D-A system and ultra-thin nanosheet structure. Density functional theory calculations further demonstrate that MB donates electrons to tri-s-triazine rings (electron acceptor). Moreover, the highest occupied molecular orbit of D-A structured g-C3N4 is mostly distributed around the MB segment, while the lowest unoccupied molecular orbit is distributed around tri-s-triazine rings, resulting in spatially separated photogenerated electron-hole pairs. Through integrating the intramolecular D-A system and ultra-thin nanosheet structure, the obtained photocatalyst exhibits enhanced charge carrier separation, an extended absorption edge, and enlarged specific surface area. As a consequence, the D-A structured g-C3N4 nanosheet shows a considerably improved photocatalytic hydrogen production activity (2275.6 μmol·h−1·g−1), which is 5.30, 2.60, and 1.30 times that of bulk g-C3N4, D-A structured bulk g-C3N4, and g-C3N4 nanosheet, respectively. This work offers a valuable strategy for developing D-A-modified photocatalytic materials for solar energy conversion.
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