Citation: Yiwen Chen, Lingling Li, Quanlong Xu, Düren Tina, Jiajie Fan, Dekun Ma. Controllable Synthesis of g-C3N4 Inverse Opal Photocatalysts for Superior Hydrogen Evolution[J]. Acta Physico-Chimica Sinica, ;2021, 37(6): 200908. doi: 10.3866/PKU.WHXB202009080 shu

Controllable Synthesis of g-C3N4 Inverse Opal Photocatalysts for Superior Hydrogen Evolution

  • Corresponding author: Quanlong Xu, xuql@wzu.edu.cn Jiajie Fan, fanjiajie@zzu.edu.cn Dekun Ma, dkma@wzu.edu.cn
  • These authors contribute equally.
  • Received Date: 25 September 2020
    Revised Date: 16 October 2020
    Accepted Date: 16 October 2020
    Available Online: 22 October 2020

    Fund Project: the Foundation of National Nature Science Foundation of China 21905209the Foundation of National Nature Science Foundation of China 21673160the Foundation of National Nature Science Foundation of China 52073263Zhejiang Provincial Natural Science Foundation of China for Distinguished Young Scholars LR16B010002China Scholarship Council 201907045030

  • The growing frustration from facing energy shortages and unbalanced environmental issues has obstructed the long-term development of human society. Semiconductor-based photocatalysis, such as water splitting, transfers solar energy to storable chemical energy and is widely considered an economic and clean solution. Although regarded as a promising photocatalyst, the low specific surface area of g-C3N4 crucially restrains its photocatalytic performance. The macro-mesoporous architecture provides effective channels for mass transfer and full-light utilization and improved the efficiency of the photocatalytic reaction. Herein, g-C3N4 with an inverse opal (IO) structure was rationally fabricated using a well-packed SiO2 template, which displayed an ultrahigh surface area (450.2 m2·g-1) and exhibited a higher photocatalytic H2 evolution rate (21.22 μmol·h-1), almost six times higher than that of bulk g-C3N4 (3.65 μmol·h-1). The IO g-C3N4 demonstrates better light absorption capacity than bulk g-C3N4, primarily in the visible spectra range, owing to the multiple light scattering effect of the three-dimensional (3D) porous structure. Meanwhile, a lower PL intensity, longer emission lifetime, smaller Nyquist semicircle, and stronger photocurrent response (which synergistically give rise to the suppressed recombination of charge carriers) decrease the interfacial charge transfer resistance and boost the formation of photogenerated electron-hole pairs. Moreover, the existing N vacancies intensify the local electron density, helping increase the number of photoexcitons. The N2 adsorption-desorption test revealed the existence of ample mesopores and macropores and high specific surface area in IO g-C3N4, which exposes more active edges and catalytic sites. Optical behavior, electron paramagnetic resonance, and electrochemical characterization results revealed positive factors, including enhanced light utilization, improved photogenerated charge separation, prolonged lifetime, and fortified IO g-C3N4 with excellent photocatalytic performance. This work provides an important contribution to the structural design and property modulation of photocatalysts.
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