Citation: Kai-Xuan XU, Yu-Long KANG, Hong-Bin HE, Xiao-Ming GAO, Chen-Yu ZHAO, Rui-Yang REN. Nitrogen-vacancies g-C₃N₅ modified S-doping perylene diimide for the enhanced visible photo self-Fenton reaction for phenol oxidation coupled with Cr(Ⅵ) reduction[J]. Chinese Journal of Inorganic Chemistry, ;2023, 39(1): 32-44. doi: 10.11862/CJIC.2022.264 shu

Nitrogen-vacancies g-C₃N₅ modified S-doping perylene diimide for the enhanced visible photo self-Fenton reaction for phenol oxidation coupled with Cr(Ⅵ) reduction

Department of Chemistry and Chemical Engineering, Clean Utilization of Low-Rank Coal of Shaanxi Collaborative Innovation Center, Shaanxi Key Laboratory of Chemical Reaction Engineering, Yan'an University, Yan'an, Shaanxi 716000, China

Corresponding author: Xiao-Ming GAO, ydgaoxm@126.com
Received Date: 31 May 2022
Revised Date: 5 October 2022

Figures(11)

Nitrogen-vacancies g-C₃N₅ (NVs) modified S-doping perylene diimide (S-PDI) organic compound semiconductor was prepared by electrostatic self-assembly. The nitrogen vacancies provided rich active sites on the surface of g-C₃N₅. The amide in the preparation of S-PDI enhanced the intermolecular interaction between S-PDI and NVs. The reduction rate of Cr(Ⅵ) over 30% NVs/S-PDI (with NVs mass fraction of 30%) was 79.96%, and the degradation rate of phenol was 74.40%. Furthermore, In the process of synergistic oxidation of phenol and reduction of Cr(Ⅵ) over 30% NVs/S-PDI, the reduction rate of Cr(Ⅵ) was 92.83%, and the degradation rate of phenol was 93.89%. Carboxylic acid and propanol, the products of oxidative degradation of phenol could be used as sacrificial agents of Cr(Ⅵ), which promoted the reduction of Cr(Ⅵ). The reduction of Cr(Ⅵ) enhanced the oxidative degradation of phenol. Accordingly, the carboxylic acid and propanol were finally oxidized to CO₂ and H₂O. Using the reduction performance of the conduction band and the oxidation performance of the valence band, the spatial separation of electrons and holes could be achieved by constructing heterojunction NVs/S-PDI, which could synergistically strengthen the oxidation half-reaction and reduction half-reaction in the photocatalytic process, simultaneously improve the photocatalytic oxidation-reduction performance. At the same time, under the illumination of visible light, H₂O₂ and Cr(Ⅵ)were generated in the phenol aqueous solution. A photo self-Fenton reaction process was formed by the electrons, H₂O₂ and Cr(Ⅵ), which further promoted the oxidative degradation of phenol and the reduction and removal of Cr(Ⅵ).
- nitrogen-vacancies g-C₃N₅,
- S-doping perylene diimide,
- photocatalysis,
- oxidation half-reaction,
- reduction half-reaction,
- photo self-Fenton reaction
1. [1]
  Liang L, Shi L, Wang F X, Wang H H, Yan P Q, Cong Y F, Yao L Z, Yang Z X, Qi W. g-C₃N₄ nano-fragments as highly efficient hydrogen evolution photocatalysts: Boosting effect of nitrogen vacancy[J]. Appl. Catal. A-Gen., 2020,599117618. doi: 10.1016/j.apcata.2020.117618
2. [2]
  Kong L R, Mu X J, Fan X M, Li R, Zhang Y T, Song P, Ma F C, Sun M T. Site-selected N-vacancy of g-C₃N₄ for photocatalysis and physical mechanism[J]. Appl. Mater. Today, 2018,13:329-338. doi: 10.1016/j.apmt.2018.10.003
3. [3]
  Ei Fakir A A, Anfar Z, Amedlous A, Zbair M, Hafidi Z, Ei Achouri M, Jada A, Ei Alem N. Engineering of new hydrogel beads based conducting polymers: Metal-free catalysis for highly organic pollutants degradation[J]. Appl. Catal. B-Environ., 2021,286119948. doi: 10.1016/j.apcatb.2021.119948
4. [4]
  Ragab E, Shaban M, Khalek A A, Mohamed F. Design and characterization of PANI/starch/Fe₂O₃ BiO composite for wastewater remediation[J]. Int. J. Biol. Macromol., 2021,181:301-312. doi: 10.1016/j.ijbiomac.2021.03.043
5. [5]
  Gao X M, Gao K L, Li X B, Shang Y Y, Fu F. Hybrid PDI/BiOCl heterojunction with enhanced interfacial charge transfer for a full-spectrum photocatalytic degradation of pollutants[J]. Catal. Sci. Technol., 2020,10(2):372-381. doi: 10.1039/C9CY01722D
6. [6]
  Gong Y B, Chang K, Chen C, Han M M, Zhan X J, Min J, Jiao X C, Li Q Q, Li Z. Pyrene-fused PDI based ternary solar cells: High power conversion efficiency over 10%, and improved device thermal stability[J]. Mater. Chem. Front., 2019,3(1):93-102. doi: 10.1039/C8QM00486B
7. [7]
  Cai Z Q, Huang Y N, Ji H D, Liu W, Fu J, Sun X B. Type-Ⅱ surface heterojunction of bismuth-rich Bi₄O ₅Br₂ on nitrogen-rich g-C₃N₅ nanosheets for efficient photocatalytic degradation of antibiotics[J]. Sep. Purif. Technol., 2022,280119772. doi: 10.1016/j.seppur.2021.119772
8. [8]
  Vadivel S, Hariganesh S, Paul B, Rajendran S, Habibi-Yangjeh A, Maruthamani D, Kumaravel M. Synthesis of novel AgCl loaded g-C₃N₅ with ultrahigh activity as visible light photocatalyst for pollutants degradation[J]. Chem. Phys. Lett., 2020,738136862. doi: 10.1016/j.cplett.2019.136862
9. [9]
  Saravanakumar K, Maheskumar V, Yea Y, Yoon Y, Muthuraj V, Park C M. 2D/2D nitrogen-rich graphitic carbon nitride coupled Bi₂WO₆ S-scheme heterojunction for boosting photodegradation of tetracycline: Influencing factors, intermediates, and insights into the mechanism[J]. Compos. Part B-Eng., 2022,234109726. doi: 10.1016/j.compositesb.2022.109726
10. [10]
  Zhang Z J, Chen X J, Zhang H J, Liu W X, Zhu W, Zhu Y F. A highly crystalline perylene imide polymer with the robust built-in electric field for efficient photocatalytic water oxidation[J]. Adv. Mater., 2020,32(32)1907746. doi: 10.1002/adma.201907746
11. [11]
  Usta H, Facchetti A, Marks T. n-Channel semiconductor materials design for organic complementary circuits[J]. Acc. Chem. Res., 2011,44:501-510. doi: 10.1021/ar200006r
12. [12]
  Wang R, Wu J, Mao X, Wang J M, Liu Q Z, Qi Y F, He P, Qi X M, Liu G L, Guan Y. Bi spheres decorated g-C₃N₄/BiOI Z-scheme het-erojunction with SPR effect for efficient photocatalytic removal elemental mercury[J]. Appl. Surf. Sci., 2021,556149804. doi: 10.1016/j.apsusc.2021.149804
13. [13]
  Li M X, Lu Q J, Liu M L, Yin P, Wu C Y, Li H T., Zhang Y Y, Yao S Z. Photoinduced charge separation via the double-electron transfer mechanism in nitrogen vacancies g-C₃N ₅/BiOBr for the photoelectro-chemical nitrogen reduction[J]. ACS Appl. Mater. Interfaces, 2020,12(34):38266-38274. doi: 10.1021/acsami.0c11894
14. [14]
  Luo J, Fan C Z, Tang L, Liu Y N, Gong Z X, Wu T S, Zhen X L, Feng C Y, Feng H P, Wang L L, Xu L, Yan M. Reveal Brønsted-Evans-Polanyi relation and attack mechanisms of reactive oxygen species for photocatalytic H₂O₂ production[J]. Appl. Catal. B-Environ., 2022,301120757. doi: 10.1016/j.apcatb.2021.120757
15. [15]
  Li H Y, Wang C, Bai X J, Wang X Y, Sun B X, Li D, Zhao L C, Zong R L, Hao D. In-plane polarization induced by the hydrogen bonding and π-π stacking of functionalized PDI supramolecules for the efficient photocatalytic degradation of organic pollutants[J]. Mater. Chem. Front., 2020,4(9):2673-2687. doi: 10.1039/D0QM00349B
16. [16]
  Hu C, Lin Y H, Yoshida M, Ashimura S. Influence of phosphorus doping on triazole-based g-C₃N₅ nanosheets for enhanced photoelec-trochemical and photocatalytic performance[J]. ACS Appl. Mater. Interfaces, 2021,13(21):24907-24915. doi: 10.1021/acsami.1c05162
17. [17]
  Wang L B, Li M H, Zhang Q, Li F Y, Xu L. Constructing electron transfer pathways and active centers over W₁₈O₄₉ nanowires by doping Fe³⁺ and incorporating g-C₃N₅ for enhanced photocatalytic nitro-gen fixation[J]. Inorg. Chem. Front., 2021,8(14):3566-3575. doi: 10.1039/D1QI00503K
18. [18]
  Zhang Y Z, Shi J W, Huang Z X, Guan X J, Zong S C, Cheng C, Zheng B T, Guo L J. Synchronous construction of CoS ₂ in-situ load-ing and doping for g-C₃N₄: Enhanced photocatalytic H₂-evolution activity and mechanism insight[J]. Chem. Eng. J., 2020,401126135. doi: 10.1016/j.cej.2020.126135
19. [19]
  LI X B, LIU J Y, HUANG J T, HE C Z, FENG Z J, CHEN Z, WAN L Y, DENG F. All organic S-scheme heterojunction PDI/S-g-C₃N₄ photocatalyst with enhanced photocatalytic performance[J]. Acta Phys.-Chim. Sin., 2021,37(6)2010030.
20. [20]
  Jiang R R, Lu G H, Nkoom M, Yan Z H, Wu D H, Liu J C, Dang T J. Mineralization and toxicity reduction of the benzophenone-1 using 2D/2D Cu₂WS ₄/BiOCl Z-scheme system: Simultaneously improved visible-light absorption and charge transfer efficiency[J]. Chem. Eng. J., 2020,400125913. doi: 10.1016/j.cej.2020.125913
21. [21]
  Li K, Cai W, Zhang Z C, Xie H F, Zhong Q, Qu H X. Boron doped C₃N₅ for photocatalytic nitrogen fixation to ammonia: The key role of boron in nitrogen activation and mechanism[J]. Chem. Eng. J., 2022,435135017. doi: 10.1016/j.cej.2022.135017
22. [22]
  Al-Hamdi A M, Sillanpää M, Bora T, Dutta J. Efficient photocatalytic degradation of phenol in aqueous solution by SnO₂: Sb nanoparticles[J]. Appl. Surf. Sci., 2016,370:229-236. doi: 10.1016/j.apsusc.2016.02.123
23. [23]
  Ishikawa A, Takata T, Kondo J N, Hara M, Kobayashi H, Domen K. Oxysulfide Sm ₂Ti₂S ₂O ₅ as a stable photocatalyst for water oxidation and reduction under visible light irradiation (λ ≤650 nm)[J]. J. Am. Chem. Soc., 2002,124:13547-13553. doi: 10.1021/ja0269643
24. [24]
  Zhang H X, Nengzi L C, Wang Z J, Zhang X Y, Li B, Cheng X W. Construction of Bi₂O₃/CuNiFe LDHs composite and its enhanced photocatalytic degradation of lomefloxacin with persulfate under simulated sunlight[J]. J. Hazard. Mater., 2020,383121236. doi: 10.1016/j.jhazmat.2019.121236
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沈阳化工大学材料科学与工程学院沈阳 110142

Nitrogen-vacancies g-C3N5 modified S-doping perylene diimide for the enhanced visible photo self-Fenton reaction for phenol oxidation coupled with Cr(Ⅵ) reduction

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通讯作者: 陈斌, bchen63@163.com

Nitrogen-vacancies g-C₃N₅ modified S-doping perylene diimide for the enhanced visible photo self-Fenton reaction for phenol oxidation coupled with Cr(Ⅵ) reduction