Citation: Xibao Li, Jiyou Liu, Juntong Huang, Chaozheng He, Zhijun Feng, Zhi Chen, Liying Wan, Fang Deng. All Organic S-Scheme Heterojunction PDI-Ala/S-C₃N₄ Photocatalyst with Enhanced Photocatalytic Performance[J]. Acta Physico-Chimica Sinica, ;2021, 37(6): 201003. doi: 10.3866/PKU.WHXB202010030 shu

All Organic S-Scheme Heterojunction PDI-Ala/S-C₃N₄ Photocatalyst with Enhanced Photocatalytic Performance

Xibao Li ^{1, 2,,} ,
Jiyou Liu ¹ ,
Juntong Huang ¹ ,
Chaozheng He ^3,, ,
Zhijun Feng ¹ ,
Zhi Chen ¹ ,
Liying Wan ¹ ,
Fang Deng ^2,,

1.
School of Materials Science and Engineering, Nanchang Hangkong University, Nanchang 330063, China
2.
National-Local Joint Engineering Research Center of Heavy Metal Pollutants Control and Resource Utilization, Nanchang Hangkong University, Nanchang 330063, China
3.
Institute of Environmental and Energy Catalysis, School of Materials Science and Chemical Engineering, Xi'an Technological University, Xi'an 710021, China

Corresponding author: Xibao Li, lixibao@nchu.edu.cn Chaozheng He, hecz2019@xatu.edu.cn Fang Deng, 40030@nchu.edu.cn
Received Date: 15 October 2020
Revised Date: 9 November 2020
Accepted Date: 18 November 2020
Available Online: 24 November 2020
Fund Project: the National Natural Science Foundation of China 51962023the National Natural Science Foundation of China 51772140the National Natural Science Foundation of China 21603109the Natural Science Foundation of Jiangxi Province, China 20192ACBL21047the Natural Science Foundation of Jiangxi Province, China 20171ACB21033the Henan Joint Fund of the National Natural Science Foundation of China U1404216the Key Laboratory of Jiangxi Province for Persistent Pollutants Control and Resources Recycle (Nanchang Hangkong University) ES202002077

Organic photocatalysts have attracted attention owing to their suitable redox band positions, low cost, high chemical stability, and good tunability of their framework and electronic structure. As a novel organic photocatalyst, PDI-Ala (N, N'-bis(propionic acid)-perylene-3, 4, 9, 10-tetracarboxylic diimide) has strong visible-light response, low valence band position, and strong oxidation ability. However, the low photogenerated charge transfer rate and high carrier recombination rate limit its application. Due to the aromatic heterocyclic structure of g-C₃N₄ and large delocalized π bond in the planar structure of PDI-Ala, g-C₃N₄ and PDI-Ala can be tightly combined through π–π interactions and N―C bond. The band structure of sulfur-doped g-C₃N₄ (S-C₃N₄) matched well with PDI-Ala than that with g-C₃N₄. The electron delocalization effect, internal electric field, and newly formed chemical bond jointly promote the separation and migration of photogenerated carriers between PDI-Ala and S-C₃N₄. To this end, a novel step-scheme (S-scheme) heterojunction photocatalyst comprising organic semiconductor PDI-Ala and S-C₃N₄ was prepared by an in situ self-assembly strategy. Meanwhile, PDI-Ala was self-assembled by transverse hydrogen bonding and longitudinal π–π stacking. The crystal structure, morphology, valency, optical properties, stability, and energy band structure of the PDI-Ala/S-C₃N₄ photocatalysts were systematically analyzed and studied by various characterization methods such as X-ray diffraction, transmission electron microscopy, energy dispersive X-ray spectrometry, X-ray photoelectron spectroscopy, ultraviolet visible diffuse reflectance spectroscopy, electrochemical impedance spectroscopy, and Mott-Schottky curve. The work functions and interface coupling characteristics were determined using density functional theory. The photocatalytic activities of the synthesized photocatalyst for H₂O₂ production and the degradation of tetracycline (TC) and p-nitrophenol (PNP) under visible-light irradiation are discussed. The PDI-Ala/S-C₃N₄ S-scheme heterojunction with band matching and tight interface bonding accelerates the intermolecular electron transfer and broadens the visible-light response range of the heterojunction. In addition, in the processes of the PDI-Ala/S-C₃N₄ photocatalytic degradation reaction, a variety of active species (h⁺, ·O₂^-, and H₂O₂) were produced and accumulated. Therefore, the PDI-Ala/S-C₃N₄ heterojunction exhibited enhanced photocatalytic performance in the degradation of TC, PNP, and H₂O₂ production. Under visible-light irradiation, the optimum 30%PDI-Ala/S-C₃N₄ removed 90% of TC within 90 min. In addition, 30%PDI-Ala/S-C₃N₄ displayed the highest H₂O₂ evolution rate of 28.3 μmol·h^-1·g^-1, which was 2.9 and 1.6 times higher than those of PDI-Ala and S-C₃N₄, respectively. These results reveal that the all organic photocatalyst comprising PDI-based supramolecular and S-C₃N₄ can be efficiently applied for the degradation of organic pollutants and production of H₂O₂. This work not only provides a novel strategy for the design of all organic S-scheme heterojunctions but also provides a new insight and reference for understanding the structure–activity relationship of heterostructure catalysts with effective interface bonding.
- Visible light photocatalysis,
- Step-scheme heterojunction,
- C₃N₄,
- π–π interactions,
- H₂O₂
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通讯作者: 陈斌, bchen63@163.com

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沈阳化工大学材料科学与工程学院沈阳 110142

All Organic S-Scheme Heterojunction PDI-Ala/S-C3N4 Photocatalyst with Enhanced Photocatalytic Performance

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通讯作者: 陈斌, bchen63@163.com

All Organic S-Scheme Heterojunction PDI-Ala/S-C₃N₄ Photocatalyst with Enhanced Photocatalytic Performance