还原氧化石墨烯基三聚氰胺海绵的制备与吸附性能

doi:10.7503/cjcu20140476

摘要/Abstract

摘要：

以天然石墨为原料, 用Hummers法和超声剥离法制备了氧化石墨烯(GO). 将氧化石墨烯浸渍, 涂覆于三聚氰胺海绵表面, 在线还原制得还原氧化石墨烯基三聚氰胺海绵(RGOME). 通过扫描电子显微镜(SEM)、傅里叶变换红外光谱(FTIR)仪及光学接触角测定仪等分析了RGOME的结构, 考察了RGOME对多种油品的吸附性能, 并对其油水选择吸附性能和循环使用性能进行了研究. 结果表明, RGOME具有疏水超亲油性, 对油品的吸附量达到56~127 g/g, 可用Bangham方程描述RGOME对甲苯和煤油的吸附动力学过程; 在选择吸附过程中, 油品浓度急剧降低, 吸附量不断升高, 分离效率达到74.49%, 可较好地实现油水分离; 吸附油品的RGOME经脱附可多次循环使用.

关键词: 还原氧化石墨烯基三聚氰胺海绵, 吸附性能, 油水分离, 疏水超亲油性

Abstract:

Graphene oxide(GO) was synthesized via the Hummers method and ultrasonic stripping method using the natural graphite as raw materials. Furtherly, reduced graphene oxide-based melamine sponges(RGOME) were fabricated via a dip-coating method which were post-reduced online. As-prepared RGOME sponges were investigated by scanning electron microscopy(SEM), Fourier transform infrared spectroscopy(FTIR) and optical contact angle measuring apparatus. Oil adsorption capacity, the oil/water selective adsorption and reusability of the RGOME sponges were also studied. The results demonstrate that the RGOME sponges exhibit good hydrophobicity and superoleophilicity, and oil adsorption capacity is up to 56—127 g/g. The adsorptive process of oils, like toluene and kerosene, was fitted to the Bangham equation for the isothermal adsorption. In terms of selective adsorptive process, the concentration of oil in oil-water mixture decreased drastically, while oil adsorption capacity constantly increased. The resulting separation efficiency was up to 74.49%, and as-prepared sponges have better performance for oil/water separation than other sorbents reported in the literature. In addition, the RGOME sponges can be reused more than 10 times with gently deteriorating in adsorption capacity.

Key words: Reduced graphene oxide-based melamine sponge, Adsorption property, Oil/water separation, Hydrophobicity and superoleophilicity

中图分类号:

O647

TrendMD:

王子涛, 肖长发, 赵健, 胡霄, 徐乃库. 还原氧化石墨烯基三聚氰胺海绵的制备与吸附性能. 高等学校化学学报, 2014, 35(11): 2410.

WANG Zitao, XIAO Changfa, ZHAO Jian, HU Xiao, XU Naiku. Preparation of Reduced Graphene Oxide-based Melamine Sponge and Its Absorption Properties^†. Chem. J. Chinese Universities, 2014, 35(11): 2410.

图/表 11

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Sorbent	Oil	Q/(g·g^-1)	Ref.	Sorbent	Oil	Q/(g·g^-1)	Ref.
RGOME	Toluene	69.8	This paper	Polypropylene nonwoven	Diesel	<8	[9]
	Trichloroethylene	127.0	This paper	Copolymerization of methyl	Toluene	<9	[8]
	Kerosene	59.3	This paper	acrylate fiber	Trichloroethylene	<21	[8]
Cotton grass fiber	Gasoline	20	[3]	Exfoliate graphite	Heavy oil	75	[38]
Corn stalk	Gasoline	8	[37]	Carbon aerogel	Toluene	130	[39]
Modified PU foam	Toluene	62	[5]		Chloroform	110	[39]
	Kerosene	47	[5]	Spongy graphene	Toluene	55	[19]
Polypropylene nonwoven	Toluene	<8	[9]		Kerosene	45	[19]

Sorbent	Oil	Q/(g·g^-1)	Ref.	Sorbent	Oil	Q/(g·g^-1)	Ref.
RGOME	Toluene	69.8	This paper	Polypropylene nonwoven	Diesel	<8	[9]
	Trichloroethylene	127.0	This paper	Copolymerization of methyl	Toluene	<9	[8]
	Kerosene	59.3	This paper	acrylate fiber	Trichloroethylene	<21	[8]
Cotton grass fiber	Gasoline	20	[3]	Exfoliate graphite	Heavy oil	75	[38]
Corn stalk	Gasoline	8	[37]	Carbon aerogel	Toluene	130	[39]
Modified PU foam	Toluene	62	[5]		Chloroform	110	[39]
	Kerosene	47	[5]	Spongy graphene	Toluene	55	[19]
Polypropylene nonwoven	Toluene	<8	[9]		Kerosene	45	[19]

Oil	Pseudo-first-order kinetic equation			Pseudo-second-order kinetic equation			Bangham equation
Oil	Q_e/(g·g^-1)	K₁/s^-1	R²	Q_e/(g·g^-1)	K₂/s^-1	R²	Q_e/(g·g^-1)	K₃/s^-1	z	R²
Toluene	68.42	0.3726	0.9880	72.93	0.0089	0.9966	69.86	0.5304	0.6853	0.9980
Kerosene	53.24	0.3140	0.9929	57.00	0.0092	0.9824	53.66	0.3820	0.8475	0.9955

Oil	Pseudo-first-order kinetic equation			Pseudo-second-order kinetic equation			Bangham equation
Oil	Q_e/(g·g^-1)	K₁/s^-1	R²	Q_e/(g·g^-1)	K₂/s^-1	R²	Q_e/(g·g^-1)	K₃/s^-1	z	R²
Toluene	68.42	0.3726	0.9880	72.93	0.0089	0.9966	69.86	0.5304	0.6853	0.9980
Kerosene	53.24	0.3140	0.9929	57.00	0.0092	0.9824	53.66	0.3820	0.8475	0.9955

Oil	Q_e(Theoretical value)/(g·g^-1)	Q_e(Experiment value)/(g·g^-1)	Relative error(%)
Toluene	68.42	69.77	1.9
Kerosene	53.24	53.82	1.0