Cu2O微晶的可控制备及可见光催化亚甲基蓝降解性能

doi:10.7503/cjcu20150091

摘要/Abstract

摘要：

以醋酸铜为铜源, 柠檬酸钠为形貌导向剂, 乙二醇和水为溶剂, 采用溶剂热法制备了立方状形貌的Cu₂O微晶. 利用X射线衍射(XRD)、 X射线光电子能谱( XPS)、扫描电子显微镜(SEM)、透射电子显微镜(TEM)和紫外-可见漫反射光谱(UV-Vis DRS)等对Cu₂O微晶进行了表征. 结果表明, 在柠檬酸钠与醋酸铜摩尔比为1.0时, 于180 ℃反应5 h可以制备出尺寸分布在0.6~1.5 μm间的均一立方状形貌Cu₂O微晶. 研究了该微晶对亚甲基蓝(MB)在可见光下降解反应的光催化性能. 结果表明, 在H₂O₂存在下, Cu₂O微晶(0.3 g/L)在100 min内对30 mg/L MB溶液的降解率可以达到98%. 该催化剂经过8次循环使用对MB的降解率仍保持在96%以上, 展现了较高的催化活性及良好的稳定性. 通过活性物种的分析对催化体系的光催化机理进行了推测.

关键词: 氧化亚铜, 溶剂热法, 光催化, 亚甲基蓝

Abstract:

Cuprous oxide microcubes were prepared by solvothermal method in glycol and water medium using copper acetate as copper source, citrate as a shape directing agent. The samples were characterized by X-ray powder diffraction(XRD), X-ray photoelectron spectroscopy(XPS), scanning electron microscopy(SEM), transmission electron microscopy(TEM) and UV-Vis diffuse reflectance spectroscopy(UV-Vis DRS). The results indicate that uniform cubic Cu₂O microcrystals with the size of 0.6—1.5 μm were synthesized at 180 ℃ for 5 h by controlling the molar ratio of sodium citrate to copper acetate. The visible-driven photocatalytic activity of Cu₂O microcrystals toward the degradation of methylene blue(MB) was investigated. The results show that after 100 min visible light irradiation, the degradation rate of methylene blue with initial concentration of 30 mg/L reached 98% by using 0.3 g/L Cu₂O microcrystals in the presence of H₂O₂. The decomposition rate of MB was still above 96% even after 8 recycling uses, thus Cu₂O microcrystals show high catalytic activity and excellent stability. The photocatalytic mechanism was discussed based on the active species during photocatlytic process.

Key words: Cu2O, Solvothermal method, Photocatalysis, Methylene blue(MB)

中图分类号:

O643.3

TrendMD:

李锋, 王桂燕, 张岩, 李洪仁. Cu₂O微晶的可控制备及可见光催化亚甲基蓝降解性能. 高等学校化学学报, 2015, 36(7): 1351.

LI Feng, WANG Guiyan, ZHANG Yan, LI Hongren. Controllable Preparation of Cu₂O Microcrystals and Their Visible-light Photocatalytic Activity Toward Degradation of Methylene Blue^†. Chem. J. Chinese Universities, 2015, 36(7): 1351.

图/表 9

Fig.1 XRD patterns of Cu2O samples

Fig.2 XPS spectra of Cu2O-1.0(A) Full spectrum; (B) Cu2p spectrum; (C) C1s spectrum.

Fig.3 SEM(A—C) and TEM(D) images of Cu2O samples(A) Cu2O-0.3; (B), (D) Cu2O-1.0; (C) Cu2O-2.0.

Fig.4 UV-Vis DR spectra of Cu2O-0.3(a),Cu2O-1.0(b) and Cu2O-2.0(c)

Fig.5 UV-Vis absorption spectra of catalytic degradation of MB with Cu2O-1.0

Fig.6 Comparison of photocatalytic activity for MB with different catalysts(A) and kinetic plot of MB photodegradation using Cu2O-1.0+H2O2 catalyst(B)(A) a. Cu2O-1.0; b. Cu2O-0.3 +H2O2; c. Cu2O-1.0 +H2O2; d. Cu2O-2.0 +H2O2.

Fig.7 Stability test of the prepared Cu2O-1.0 microcrystals in photodegradation of MB

Fig.8 Repeated cyclic voltammograms of Cu2O-modified glassy carbon electrode

Fig.9 Fluorescence spectral changes under visible light irradiation with increasing time for the Cu2O-1.0+H2O2 in coumarin aqueous solution(A) and effects of scavenger on photodegradation of MB(B)

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Cu₂O微晶的可控制备及可见光催化亚甲基蓝降解性能

Controllable Preparation of Cu₂O Microcrystals and Their Visible-light Photocatalytic Activity Toward Degradation of Methylene Blue^†

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