有序介孔三氧化二铟/还原氧化石墨烯纳米复合材料的制备及可见光催化性能

doi:10.7503/cjcu20140733

摘要/Abstract

摘要：

以有序介孔三氧化二铟(m-In₂O₃)和还原氧化石墨烯(RGO)为原料, 采用紫外光照射法合成了介孔三氧化二铟/还原氧化石墨烯(m-In₂O₃-RGO)复合光催化剂. 利用N₂吸附-脱附、 X射线衍射(XRD)、透射电子显微镜(TEM)、漫反射吸收光谱(DRS)和光电流测试等手段对样品进行表征. 在可见光照射下, 以对氯苯酚(4-CP)为目标污染物, 考察了m-In₂O₃-RGO光催化剂的催化性能. 结果表明, m-In₂O₃-RGO光催化剂具有完整的晶型和规则的孔道结构, 有利于光生电子和空穴的分离. 同时, 作为固态电子受体与传输体的RGO促进了光生电子-空穴对的传输和分离, 有效提高了可见光催化性能. 掺杂2%(质量分数)RGO的复合光催化剂性能最佳, 4 h可将4-CP降解96%以上, 催化剂经多次循环使用后, 其光催化活性基本保持不变.

关键词: 介孔三氧化二铟, 还原氧化石墨烯, 纳米复合物, 可见光催化

Abstract:

Ordered mesoporous indium dioxide(m-In₂O₃)/reduced graphene oxide(RGO) nanocomposites(m-In₂O₃-RGO) were prepared by a facile UV-assisted photoreduction method. The as-prepared samples were characterized by N₂ adsorption-desorption, X-ray diffraction, transmission electron microscopy, UV-Vis diffuse reflectance spectroscopy and photocurrent techniques. Photocatalytic properties of m-In₂O₃-RGO nanocompo-site were studied under different conditions by using 4-chlorophenol(4-CP) as target pollutant under visible light irradiation. The results indicate that m-In₂O₃-RGO nanocomposite equip with high crystallinity and continuous pore channels, which provide a short distance for photogenerated charge carriers transfer. Simulta-neously, RGO acts herein as a solid-state electron mediator, promoting the charge transportation and separation, as well as suppressing the electron-hole recombination in the composite. Under visible light irradiation, the photodegradation rate of 4-CP from the optimized photocatalyst containing ca. 2%(mass fraction) RGO reached to 96%. Meanwhile, the photocatalyst could be recycled several times without losing its photocatalytic performance.

Key words: Mesoporous indium dioxide, Reduced graphene oxide, Nanocomposite, Visible light photocatalysis

中图分类号:

O643

TrendMD:

丁敏娟, 黄徽, 杨平. 有序介孔三氧化二铟/还原氧化石墨烯纳米复合材料的制备及可见光催化性能. 高等学校化学学报, 2015, 36(5): 989.

DING Minjuan, HUANG Hui, YANG Ping. Preparation and Visible Light Photocatalytic Performance of Ordered Mesoporous Indium Dioxide/Reduced Graphene Oxide Nanocomposite^†. Chem. J. Chinese Universities, 2015, 36(5): 989.

图/表 12

Fig.1 N2 absorption-desorption isothermal of the m-In2O3(a) and m-In2O3-RGO(b) photocatalysts

Fig.2 Pore diameter distribution of the m-In2O3(a) and m-In2O3-RGO(b) photocatalysts

Table 1 Pore structure parameters of the of KIT-6, m-In2O3 and m-In2O3-RGO samples

Sample	$S BET$ /(m²·g^-1)	$V T$ /(cm³·g^-1)	d₀/nm
KIT-6	633.5	1.636	8.16
m-In₂O₃	131.5	0.35	3.95
m-In₂O₃-RGO-2%	141.2	0.40	4.03

Table 1 Pore structure parameters of the of KIT-6, m-In2O3 and m-In2O3-RGO samples

Sample	$S BET$ /(m²·g^-1)	$V T$ /(cm³·g^-1)	d₀/nm
KIT-6	633.5	1.636	8.16
m-In₂O₃	131.5	0.35	3.95
m-In₂O₃-RGO-2%	141.2	0.40	4.03

Fig.3 XRD patterns of In2O3(a), m-In2O3(b) and m-In2O3-RGO(c) photocatalysts

Fig.4 TEM(A), SEM(B), HRTEM(C, D) images and SAED(E), EDX(F) patterns of m-In2O3(A, B) and m-In2O3-RGO(C―F) photocatalyst

Fig.5 FTIR spectra of GO(a) and m-In2O3-RGO(b) composite

Fig.6 UV-Visible diffuse absorption spectrum of m-In2O3 and m-In2O3-RGO-x photocatalystsa. m-In2O3; b. m-In2O3-RGO-1%; c. m-In2O3-RGO-2%; d. m-In2O3-RGO-5%; e. m-In2O3-RGO-7%; f. m-In2O3-RGO-10%.

Fig.7 Photocurrents of m-In2O3(a), m-In2O3-RGO-1%(b), m-In2O3-RGO-2%(c), m-In2O3-RGO-5%(d), m-In2O3-RGO-7%(e) and m-In2O3-RGO-10%(f) samples under visible light irradiation(λ>420 nm) at a bias potential of 1.2 V

Fig.8 Effect of RGO amount on photodegradation rate of 4-CP at pH=3 a. c-In2O3; b. m-In2O3; c. m-In2O3-RGO-1%;d. m-In2O3-RGO-2%; e. m-In2O3-RGO-5%;f. m-In2O3-RGO-7%; g. m-In2O3-RGO-10%.

Fig.9 Effect of pH values on the photodegradation rate of 4-CP with m-In2O3-RGO-2% as catalyst

Fig.10 Effect of recycle times on photodegradation rate of 4-CP with m-In2O3-RGO-2% as catalyst at pH=3

Fig.11 Reaction mechanism of m-In2O3-RGO photocatalysts for photodegradation of 4-CP

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