Hydrochloric acid-mediated synthesis of ZnFe2O4 small particle decorated one-dimensional Perylene Diimide S-scheme heterojunction with excellent photocatalytic ability

doi:10.1016/S1872-2067(21)63930-X

Abstract

Abstract:

The recyclable and stable ZnFe₂O₄ small particle decorated one-dimensional perylene diimide (PDI) S-scheme heterojunction (1D PDI/ZnFe₂O₄) is prepared by the hydrochloric acid-mediated (HCl-mediated) strategy, interestingly, the morphology of the 1D PDI/ZnFe₂O₄ can also be effectively regulated by HCl-mediated process, the existence of HCl can regulate PDI into a uniform rod structure, while the co-existence of HCl and PDI can limit ZnFe₂O₄ to become the uniform small particles. More importantly, based on the 1D rod structure of PDI and the small size effect of ZnFe₂O₄, carriers can migrate to the surface more easily, which can improve the photocatalytic activity. Meanwhile, due to the appropriate energy level structure, the S-scheme heterojunction structure is formed between PDI and ZnFe₂O₄, which eliminates meaningless photo-generated charge carriers through recombination and introduces strong redox to further enhance the photodegradation effect, thereby, 1D PDI/ZnFe₂O₄ exhibits excellent photocatalytic ability, under the visible light irradiation, the degradation rate of tetracycline (TC) with 1D PDI/ZnFe₂O₄ (66.67%) is 9.18 times that with PDI (7.26%) and 9.73 times that with ZnFe₂O₄ (6.85%). This work proposes new ideas for the assembly of magnetic organic-inorganic S-scheme heterojunction photocatalysts.

Key words: Hydrochloric acid-mediated strategy, Morphology regulation, Perylene diimide/ZnFe₂O₄, S-scheme heterojunction, Photocatalytic ability

Yangrui Xu, Xiaodie Zhu, Huan Yan, Panpan Wang, Minshan Song, Changchang Ma, Ziran Chen, Jinyu Chu, Xinlin Liu, Ziyang Lu. Hydrochloric acid-mediated synthesis of ZnFe₂O₄ small particle decorated one-dimensional Perylene Diimide S-scheme heterojunction with excellent photocatalytic ability[J]. Chinese Journal of Catalysis, 2022, 43(4): 1111-1122.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(21)63930-X

https://www.cjcatal.com/EN/Y2022/V43/I4/1111

Figures/Tables 18

Scheme 1. The synthesis process of 1D PDI/ZnFe2O4 by the HCl-mediated strategy.

Fig. 1. TEM images of PDI (a), ZnFe2O4 (b), 1D PDI/ZnFe2O4 (c and d), PDI/ZnFe2O4 (e) and HCl-ZnFe2O4 (f).

Fig. 2. N2 adsorption-desorption isotherm of the PDI (a), ZnFe2O4(b) and 1D PDI/ZnFe2O4(c).

Fig. 3. XRD patterns (a) and FTIR spectra (b) of different samples.

Fig. 4. XPS spectra of 1D PDI/ZnFe2O4. (a) The survey spectra; (b) C 1s; (c) N 1s; (d) O 1s; (e) Zn 2p; (f) Fe 2p.

Fig. 5. Magnetization patterns at room temperature (a) and UV-vis diffuse reflectance spectrum of different samples (b). (inset in a is the photograph of 1D PDI/ZnFe2O4 separated from solution under a magnet).

Fig. 6. Degradation rates (a), the pseudo-first-order kinetics fitting data (b), degradation rates and error analysis of three repeated experiments at 60 min (c), the pseudo-first-order kinetics fitting data and error analysis of three repeated experiments at 60 min (d) for photodegradation of TC over different samples.

Table 1 Degradation rates and apparent rate constants for degradation of TC with different samples at 60 min and the corresponding error analysis of three repeated experiments.

Sample	Degradation rate (%)	Apparent rate constant (min^-1)
No sample	4.55 ± 0.25	0.065 ± 0.002
PDI	7.26 ± 0.35	0.16 ± 0.004
ZnFe₂O₄	6.85 ± 0.45	0.19 ± 0.004
1D PDI/ZnFe₂O₄	66.67 ± 1.8	1.10 ± 0.03
PDI/ZnFe₂O₄	7.98 ± 0.67	0.08 ± 0.007
HCl-ZnFe₂O₄	7.55 ± 0.56	0.08 ± 0.007

Fig. 7. Degradation rates and error analysis of three repeated experiments at 60 min for TC degradation with 1D PDI/ZnFe2O4 under different cycle times.

Fig. 8. The EIS plots (a) and photocurrent response (b) of different samples.

Fig. 9. Mott-Schottky plots of PDI (a) and ZnFe2O4 (b).

Fig. 10. The tauc plots of PDI (a) and ZnFe2O4 (b).

Fig. 11. Work function of PDI (a) and ZnFe2O4 (b), the structural models for DFT calculation (Inset).

Fig. 12. The effect of degradation of TC in existence of different quenchers and error analysis of three repeated experiments at 60 min over 1D PDI/ZnFe2O4 (a), and the corresponding time-change UV-vis UV-vis absorption spectrum (b-d).

Fig. 13. ESR of •O2-(a) and •OH (b) for PDI, ZnFe2O4 and 1D PDI/ZnFe2O4.

Fig. 14. The electron transfer mechanism near the interface of 1D PDI/ZnFe2O4. (a) PDI and ZnFe2O4 before contact; (b) PDI and ZnFe2O4 after contact; (c) PDI/ZnFe2O4 under light irradiation.

Fig. 15. The proposed photocatalytic mechanism of degradation of TC by 1D PDI/ZnFe2O4.

Fig. 16. The possible intermediates products on degradation of TC.

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Hydrochloric acid-mediated synthesis of ZnFe₂O₄ small particle decorated one-dimensional Perylene Diimide S-scheme heterojunction with excellent photocatalytic ability

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