氧化石墨烯-TiO2复合材料对三种染料的吸附动力学及光催化性能

doi:10.16085/j.issn.1000-6613.2018-1866

摘要/Abstract

摘要：

通过在氧化石墨烯分散溶液中水解钛酸丁酯成功制备氧化石墨烯-TiO₂复合材料（GO-TiO₂），采用傅里叶变换红外光谱（FTIR）、X射线衍射（XRD）、扫描电子显微镜（SEM）、X射线光电子能谱（XPS）、全自动比表面及孔径分析仪（BET）和紫外-可见漫反射光谱（UV-vis DRS）等对样品进行了表征。研究了GO10-TiO₂对亚甲基蓝（MB）、甲基橙（MO）和罗丹明B（RhB）3种染料的吸附动力学和光催化性能。结果表明：TiO₂颗粒均匀地附着在GO片层表面；GO10-TiO₂对3种染料的吸附过程为多层吸附，吸附动力学符合拟二级动力学模型；在25℃条件下GO10-TiO₂对废水中MB、MO和Rh B的吸附因共轭结构、极性等的差异而呈现选择性吸附，吸附容量分别为9.2mg/g、5.4mg/g和23.0mg/g。对3种染料废水的光催化降解效果与吸附性能相关联，吸附容量越大降解效率越高，光催化反应60min时，MB、MO和Rh B降解率分别为89%、75%和98%。

关键词: 氧化石墨烯, 二氧化钛, 等温吸附曲线, 吸附动力学, 光催化反应

Abstract:

The titania-loaded graphene oxide composites (GO-TiO₂) were prepared by hydrolysis of butyl titanate in graphene oxide dispersed solution. The modified samples were characterized by Fourier transform infrared (FTIR), X-ray diffraction (XRD), scanning electron microscopy (SEM), X-ray photoelectron spectroscopy (XPS), automatic specific surface area and pore analysis (BET), and UV-vis diffuse spectroscopy (UV-vis DRS). The adsorption kinetics and photocatalytic properties of GO10-TiO₂ for methylene blue (MB), methyl orange (MO) and Rhodamine B (Rh B) dyes were studied. The results showed that the TiO₂ particles were uniformly attached to the surface of GO sheet, the adsorption process of GO10-TiO₂ for three dyes was multi-layer adsorption, and the adsorption kinetics accords with the pseudo-second-order kinetic model. At 25℃, the adsorption of MB, MO and Rh B in wastewater by GO10-TiO₂ showed selective adsorption due to the difference of conjugate structure and polarity with adsorption capacities of 9.2mg/g, 5.4mg/g and 23.0mg/g, respectively. The photocatalytic degradation of the three dye wastewaters was related to the adsorption performance. The higher the adsorption capacity, the higher the degradation efficiency. The degradation rates of MB, MO and Rh B were 89%, 75% and 98%, respectively, after photocatalytic reaction for 60min.

Key words: graphene oxide, titanium dioxide, isothermal adsorption curve, adsorption kinetics, photocatalytic reaction

中图分类号:

TQ174

张巧玲, 秦钊, 刘有智, 师艳婷, 张竞文, 曾广平. 氧化石墨烯-TiO₂复合材料对三种染料的吸附动力学及光催化性能[J]. 化工进展, 2019, 38(06): 2870-2879.

Qiaoling ZHANG, Zhao QIN, Youzhi LIU, Yanting SHI, Jingwen ZHANG, Guangping ZENG. Adsorption kinetics and photocatalytic activity of grapheneoxide-TiO₂ composites for three dyes[J]. Chemical Industry and Engineering Progress, 2019, 38(06): 2870-2879.

图/表 17

参考文献 31

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2θ/（°）	晶面	2θ/（°）	晶面
25	（101）	62	（204）
38	（004）	69	（116）
48	（200）	70	（220）
53	（105）	75	（215）

2θ/（°）	晶面	2θ/（°）	晶面
25	（101）	62	（204）
38	（004）	69	（116）
48	（200）	70	（220）
53	（105）	75	（215）

2θ/（°）	晶面
27	（110）
55	（211）

2θ/（°）	晶面
27	（110）
55	（211）

材料	比表面积/m²·g^-1
GO	339.0
TiO₂	53.9
GO1-TiO₂	63.8
GO5-TiO₂	89.7
GO10-TiO₂	109.7
GO15-TiO₂	121.1
GO20-TiO₂	134.6

氧化石墨烯-TiO₂复合材料对三种染料的吸附动力学及光催化性能

Adsorption kinetics and photocatalytic activity of grapheneoxide-TiO₂ composites for three dyes

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参考文献 31

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复合材料	吸附率/%	60min总降解率/%
TiO₂	0	52.4
GO1-TiO₂	6.3	85.3
GO5-TiO₂	8.0	87.3
GO10-TiO₂	15.3	94.0
GO15-TiO₂	16.7	65.0
GO20-TiO₂	17.0	52.7

染料	q _m,exp /mg·g^-1	Langmuir 模型			Freundlich 模型
染料	q _m,exp /mg·g^-1	q _m,cal/mg·g^-1	K _L/L·mg^-1	R ²	K _F	n	R ²
MB	9.2	10.10	0.020	0.734	0.114	0.726	0.982
MO	5.4	2.53	0.027	0.701	0.023	0.603	0.994
Rh B	23.0	26,31	0.038	0.763	0.902	0.859	0.993

染料	q _e,exp /mg·g^-1	拟一级动力学			拟二级动力学			颗粒内扩散模型
染料	q _e,exp /mg·g^-1	q _e,cal /mg·g^-1	k ₁ /min^-1	R ²	q _e,cal /mg·g^-1	k ₂ /mg·g^-1·min^-1	R ²	k_i, ₁ /mg·g^-1·min^-1/2	k_i, ₂ /mg·g^-1·min^-1/2
MB	9.203	9.936	0.053	0.937	9.379	11.43×10^-3	0.991	1.331	0.083
MO	5.421	5.708	0.049	0.988	5.408	34.19×10^-3	0.990	0.701	0.056
Rh B	23.123	26.316	0.088	0.986	24.456	1.672×10^-3	0.997	2.042	0.102

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染料	相对分子质量	极性汉森参数δ _p
MB	319	2.904
MO	327	3.113
Rh B	479	4.298

染料	相对分子质量	极性汉森参数δ _p
MB	319	2.904
MO	327	3.113
Rh B	479	4.298