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

Yiwen Chen ^{1, †} ,
Lingling Li ^{2, †} ,
Quanlong Xu ^3,, ,
Düren Tina ⁴ ,
Jiajie Fan ^{1, 4,,} ,
Dekun Ma ^5,,

1.
School of Materials Science and Engineering, Zhengzhou University, Zhengzhou 450002, China
2.
School of Materials and Energy, Guangdong University of Technology, Guangzhou 510006, China
3.
Key laboratory of Carbon Materials of Zhejiang Province, College of Chemistry and Materials Engineering, Wenzhou University, Wenzhou 325027, Zhejiang Province, China
4.
Centre for Advanced Separations Engineering, Department of Chemical Engineering, University of Bath, Bath BA2 7AY, UK
5.
Zhejiang Key Laboratory of Alternative Technologies for Fine Chemicals Process, Shaoxing University, Shaoxing 312000, Zhejiang Province, China

Corresponding author: Quanlong Xu, xuql@wzu.edu.cn Jiajie Fan, fanjiajie@zzu.edu.cn Dekun Ma, dkma@wzu.edu.cn

^†

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.
- g-C₃N₄,
- Inverse opal (IO),
- Photocatalysis,
- H₂ evolution
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沈阳化工大学材料科学与工程学院沈阳 110142

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

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