Effect of Zn, C Introduction Amount and Calcination Temperature on the Photocatalytic Reduction of Cu2+over ZnO/C/CeO2

doi:10.6023/A24040144

Abstract

In this study, the Zn(OH)₂/AR14/Ce(OH)₄ precursor was prepared by a co-deposition method using Ce(NO₃)₃•6H₂O as the cerium source, Zn(NO₃)₂•6H₂O as the zinc source, and acidic red 14 (AR14) as the carbon source. Then, ZnO/C/CeO₂ materials were obtained by calcination of the precursor in a tube furnace under N₂ atmosphere at different temperatures. The composite was characterized by X-ray diffraction, scanning electron microscope, Fourier transform infrared spectroscopy, photoluminescence and X-ray photoelectron spectroscopy. The results showed that the ternary composites were prepared successfully, and that the carbon existed in an amorphous form. Due to the thermal decomposition of the precursor at high temperatures, the synthesized products exhibit porous property. Due to the uniform distribution of reactants in the reaction system, the distribution of Zn, Ce and C in the obtained material was uniform. It can be seen that the introduction of Zn and the formation of Ce³⁺ in CeO₂ are conducive to the formation of oxygen vacancies, generating intermediate energy levels and thus broadening the light absorption range. Furthermore, oxygen vacancies can easily capture photoelectrons and thus accelerate their separation from holes in the value band, which can improve the photocatalytic efficiency of the resulted materials. The introduction of C into CeO₂ can produce a certain amount of carbon bonds, promote the effective separation of photoelectrons and holes, and improve the photocatalytic activity of the product. The effects of the amount of introduced Zn and C and the calcination temperature on the photocatalytic activity of ZnO/C/CeO₂ were investigated by the photocatalytic reduction of Cu²⁺. The results showed that when the amount of Zn(NO₃)₂•6H₂O in the reaction raw material was 0.5 g, the concentration of AR14 was 0.05 mmol/L, and the calcination temperature was 350 ℃ for the precursor, the photocatalytic reduction efficiency of Cu²⁺ over ZnO/C/CeO₂ is the highest, reaching 95.34%. The main reasons for the best photocatalytic performance are the highest oxygen vacancy concentration and maximum number of carbon bonds in ZnO/0.05C/2CeO₂-350, resulting in the highest separation efficiency of photogenerated electrons and holes.

Key words: ZnO/C/CeO₂, Cu²⁺, photocatalytic reduction, oxygen vacancy, electron-hole pair

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Fanfan Zhang, Yuantao Cai, Jianbo Tao, Guoju Chang, Xinchen Guo, Shiyou Hao. Effect of Zn, C Introduction Amount and Calcination Temperature on the Photocatalytic Reduction of Cu²⁺over ZnO/C/CeO₂[J]. Acta Chimica Sinica, 2024, 82(8): 871-878.

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Fig. & Tab. 11

Figure 1. XRD patterns (a) and infrared spectra (c) of CeO2/0.05C-350, ZnO/0.05C-350, ZnO/2CeO2-350, ZnO/0.05C/2CeO2-350 and shifting of (111) peak for CeO2/0.05C-350, ZnO/0.05C-350, ZnO/0.05C/2CeO2-350 (b)

Figure 2. Mapping of Ce (a), Zn (b), O (c), C (d), EDS contents (e) and SEM in ZnO/0.05C/2CeO2-350 (f)

Figure 3. (a~d) Removal efficiency of Cu2+ over different catalysts and (e) removal efficiency of Cu2+ over the control and optimal samples

Figure 4. Cu 2p deconvolution XPS of ZnO/0.05C/2CeO2-350 after dark treatment (a) and photocatalysis (b)

Figure 5. Diffuse reflectance UV-Vis spectra of CeO2/0.05C-350, ZnO/0.05C-350, ZnO/2CeO2-350, ZnO/0.05C/CeO2-350, ZnO/0.05C/ 2CeO2-350, ZnO/0.05C/3CeO2-350 (a) and optical absorption edges (b)

Figure 6. Photoemission spectra (a) and photocurrent spectra (b) of CeO2/0.05C-350, ZnO/0.05C-350, ZnO/2CeO2-350, ZnO/0.01C/ 2CeO2-350, ZnO/0.05C/2CeO2-350 and ZnO/0.1C/2CeO2-350

Figure 7. Effect of temperature on the photocatalytic removal of Cu2+

Figure 8. Ce 3d deconvolution XPS spectra of ZnO/0.05C/2CeO2-350 (a), ZnO/0.05C/2CeO2-450 (b) and ZnO/0.05C/2CeO2-550 (c)

Figure 9. C 1s deconvolution XPS spectra of ZnO/0.05C/2CeO2-350 (a), ZnO/0.05C/2CeO2-450 (b) and ZnO/0.05C/2CeO2-550 (c)

Sample	Area of C=C	Area of C=O	Area of O—C=O	Total Area
ZnO/0.05C/2CeO₂-350	4882.488	825.3487	1244.586	6952.4227
ZnO/0.05C/2CeO₂-450	4496.099	401.5865	805.8344	5703.5199
ZnO/0.05C/2CeO₂-550	3459.989	893.3685	1177.464	5530.8215

Table 1. The peak area of different types of carbon bonds in different catalysts

Figure 10. O 1s deconvolution XPS spectra of ZnO/0.05C/2CeO2-350 (a), ZnO/0.05C/2CeO2-450 (b) and ZnO/0.05C/2CeO2-550 (c)

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Zn, C引入量和煅烧温度对ZnO/C/CeO₂光催化还原Cu²⁺效率的影响

Effect of Zn, C Introduction Amount and Calcination Temperature on the Photocatalytic Reduction of Cu²⁺over ZnO/C/CeO₂

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Zn, C引入量和煅烧温度对ZnO/C/CeO2光催化还原Cu2+效率的影响