超疏水、 高强度石墨烯油水分离材料的制备及应用

doi:10.7503/cjcu20180332

摘要/Abstract

摘要：

通过绿色环保的表面修饰方法, 采用氧化石墨烯(GO)对双亲的三聚氰胺海绵(MS)进行表面改性, 制备了超疏水的还原氧化石墨烯/三聚氰胺海绵(RGO-MS). 采用X射线衍射(XRD)、拉曼光谱(Raman)、傅里叶变换红外光谱(FTIR)及扫描电子显微镜(SEM)对制备的RGO-MS进行了结构、形貌和组分分析, 并对其机械性能、疏水性、吸附性能、循环使用和连续油水分离性能进行了研究. 实验结果表明, 还原氧化石墨烯涂层和海绵骨架紧密相连; RGO-MS对水上浮油和水下重油均具有优异的吸附能力, 并且在完成50次吸附-挤压循环测试之后仍保持90%以上的吸附能力, 对静止和搅拌情况下的油水混合物的分离效率分别高达4.5×10⁶和3×10⁶ L/(m³·h). 因此, RGO-MS在处理油脂和有机物泄漏造成的大面积污染方面有着巨大的应用前景.

关键词: 还原氧化石墨烯/三聚氰胺海绵, 超疏水, 吸附性能, 油水分离

Abstract:

Superhydrophobic reduced graphene oxide-wrapped melamine sponge(RGO-MS) was prepared via a facile surface modification method with graphene oxide(GO) modification amphipathic melamine sponge(MS). X-ray diffraction(XRD), Raman spectra, Fourier transform infrared spectroscopy(FTIR) and scanning electron microscopy(SEM) were used to investigate the structure, morphology and component of RGO-MS. The mechanical property, hydrophobicity, oil adsorption capacity, reusability and oil/water separation efficiency of RGO-MS were also explored. The results revealed that reduced graphene oxide(RGO) coating was closely linked to MS skeleton. In addition, RGO-MS possesses outstanding adsorption capacity for floating oil and heavy oil underwater, and could maintain ultra-high adsorption capacity even after 50 adsorption-squeezing cycles which is as high as 90 % of its initial adsorption capacity. Moreover, RGO-MS exhibits extremely high separation efficiency up to 4.5×10⁶ L/(m³·h) under non-turbulent and 3×10⁶L/(m³·h) under turbulent condition water/oil system. Therefore, RGO-MS has a huge application prospect in dealing with the large-scale removal of oil and organic spillage cleanup.

Key words: Reduced graphene oxide-wrapped melamine sponge, Superhydrophobic, Adsorption capacity, Oil/water separation

中图分类号:

O648

TrendMD:

邱丽娟, 张颖, 刘帅卓, 张骞, 周莹. 超疏水、高强度石墨烯油水分离材料的制备及应用. 高等学校化学学报, 2018, 39(12): 2758.

QIU Lijuan,ZHANG Ying,LIU Shuaizhuo,ZHANG Qian,ZHOU Ying. Preparation and Application of Superhydrophobic and Robust Graphene Composites Oil/Water Separation Material^†. Chem. J. Chinese Universities, 2018, 39(12): 2758.

图/表 13

Fig.1 XRD patterns of MS(a) and RGO-MS(b)

Fig.2 Raman(A) and FTIR spectra(B) of MS(a), GO-MS(b) and RGO-MS(c)

Fig.3 Optical images of RGO-MS prepared with watch glasses(A) and beaker(B)

Fig.4 SEM images of MS(A, D), GO-MS(B, E) and RGO-MS(C, F) after 30 squeezing and 20 twist testsInsets: the photographs of the corresponding sponges.

Fig.5 Compressive stress-strain curves of RGO-MS with different set strain of 40%, 60%, 80%, respectively(A) and cyclic compressive stress-strain curves of RGO-MS at 60% strain(B)Insets: the process of compression text(A) and the photograph of the twisted RGO-MS(B).

Fig.6 Optical images of static water droplet on the surface of MS(A) and RGO-MS(B, C) (C) Enlarged image of static water dropcet on the surface of RGO-MS.

Fig.7 Dynamic contact angles test of water droplet on RGO-MSVolume of water droplet: (A) 4 μL; (B) 7 μL; (C) 4 μL.

Table 1 Comparison of adsorption capacity of various adsorbents

Adsorbent	Contact angle/(°)	Q_wt/(g·g^-1)	Adsorption rate/(L·h^-1)	Cycle time	Ref.
RGO-MS	163±10	62—120	18	>50	This work
PEI/RGO-Polyurethane	95.82	6.9—8.8		30	[9]
RGO	114±2	20—86		>10	[17]
GO-CNT	147.6±2	21—35	6	8	[30]
PDMS-graphene	126.6	2—8	9	5	[31]
RGO	135	100—280	<6	5	[38]
Nanodiamond- Polyurethane	150±2	3—60		10	[39]
RGO-MS	154	57—112		20	[40]

Fig.8 Adsorption capacity towards oil and organic solvents over RGO-MS(A) and recycling adsorption performance towards hexane and pump oil over RGO-MS(B)Insets in (B) are the photographs of adsorption-squeezing process over RGO-MS.

Fig.9 Selective adsorption of RGO-MS for floating oil(pump oil)(A) and underwater heavy oil(phenixin)(B)

Fig.10 Change of non-turbulent floating oil liquid level in continuous oil-water separation process with RGO-MS at different time Time/s: (A) 0; (B) 5; (C) 10; (D) 20.

Fig.11 Change of turbulent floating oil liquid level in continuous oil-water separation process with RGO-MS at different time Time/s: (A) 0; (B) 5; (C) 20; (D) 30.

Fig.12 Change of heavy oil liquid level in continuous oil-water separation process with RGO-MS at different time

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