Study on Preparation of Ag/AgCl/ZIF-8 Composite and Photocatalytic NO Oxidation Performance

doi:10.6023/A22060266

Abstract

ZIF-8, a subclass of metal-organic frameworks with Zn²⁺ and 2-methylimidazole, featuring high special surface area and easily adjustable structures have exhibit great application potential in photocatalytic reaction. However, ZIF-8 often suffers from short light harvesting range and rapid recombination of photogenerated carriers, resulting in poorer catalytic activity. Here, ZIF-8 was synthesized by a precipitation method, and then Ag/AgCl nanoparticles were deposited on the surface of ZIF-8 by photo-deposition to obtain Ag/AgCl/ZIF-8 composite. The typical synthesis procedure is as follows: 0.2 g of ZIF-8 powder was dispersed in 50 mL of methanol and sonicated for 30 min to make it uniformly dispersed, then 0.1699 g of AgNO₃ (1 mmol) and 0.045 g ZnCl₂were added to the above solution, which was placed on a magnetic stirrer and stirred in the dark for 30 min, followed irradiating it under light for 10 min. The obtained sample was washed several times with methanol and dried under a freeze-drying oven for 12 h. The crystal structure, morphology, specific surface area and light absorption properties were characterized by using X-ray diffractometer (XRD), scanning electron microscope (SEM), transmission electron microscope (TEM), specific surface area test method (BET) and UV-Vis diffuse reflection absorption spectra (UV-Vis DRS), respectively. Finally, the photocatalytic oxidation performance of Ag/AgCl/ZIF-8 for NO removal under visible light was systematically studied, and its reaction mechanism was further analyzed. Thus, the resulting Ag/AgCl/ZIF-8 composite showed enhanced NO photocatalytic removal performance, reaching the highest NO removal of 43.5% under 35 min visible light irradiation and better stability compared with the parent ZIF-8. The above results show that: (1) Ag⁰ surface plasmon resonance (SPR) effect in Ag/AgCl/ZIF-8 composite enhances the absorption of visible light; (2) ZIF-8 can enrich more oxygen molecules and NO molecules, promoting the formation of superoxide free radicals and NO photocatalytic oxidation performance with a large specific surface area; (3) the photogenerated holes in the composite can be transferred to the surface of AgCl to oxidate Cl^- to Cl⁰, which possess more strong oxidation ability for improving the photocatalytic oxidation of NO. On the other hand, it effectively inhibits the recombination of photogenerated electrons and holes, which improves the stability of the catalyst.

Key words: nitrogen oxides, photocatalytic oxidation, metal organic framework materials, ZIF-8 composite

Cite this article

Pengfei Zhu, Chensi Lou, Yuhan Shi, Chuanyi Wang. Study on Preparation of Ag/AgCl/ZIF-8 Composite and Photocatalytic NO Oxidation Performance[J]. Acta Chimica Sinica, 2022, 80(10): 1385-1393.

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Fig. & Tab. 15

Figure 1. (a) XRD patterns of ZIF-8, Ag/AgCl, Ag/ZIF-8, AgCl/ZIF-8 and AACZ8-0.075; (b) the X-ray diffraction patterns of Ag/AgCl, Ag/ZIF-8 and AACZ8-0.075 were locally amplified

Figure 2. (a, b) SEM images of ZIF-8 and AACZ8-0.075; (c, d) TEM images of ZIF-8 and AACZ8-0.075

Figure 3. (a, b) HRTEM images of AACZ8-0.075

Figure 4. EDS element mappings of AACZ8-0.075

Figure 5. N2 adsorption-desorption isotherms of ZIF-8 and AACZ8-0.075

样品	比表面积/ (m²•g^-1)	孔径/nm	孔隙体积/ (cm³•g^-1)
ZIF-8	1270.4993	0.3633	0.551171
AACZ8-0.075	822.8584	0.3621	0.353376

Table 1. The specific surface area, pore size and pore volume of ZIF-8 and AACZ8-0.075 composites

Figure 6. XPS spectra of ZIF-8 and AACZ8-0.075: (a) full spectra, (b) C 1s, (c) N 1s, (d) Zn 2p, (e) Cl 2p, (f) Ag 3d

Figure 7. (a) UV-Vis absorption spectra of the samples; (b) band gap widths of ZIF-8 and AACZ8-0.075

Figure 8. Photocurrent graph of the samples (i-t) (a) and electrochemical impedance spectroscopy (EIS) of the samples

Figure 9. PL spectra of the samples

Figure 10. (a) Photocatalytic activity for the removal of NO; (b) cyclic test for the sample AACZ8-0.075

Figure 11. Free radical trapping experiment on photocatalytic NO oxidation for the sample AACZ8-0.075

Figure 12. (a) The ESR spectra of DMPO-•OH; (b) the ESR spectra of DMPO-•O2-

Figure 13. The Mott-Schottky plots of ZIF-8

Figure 14. Mechanism diagram of NO removal by AACZ8-0.075 photocatalysis

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Ag/AgCl/ZIF-8复合材料的制备及其对NO光催化氧化性能的研究