使用非离子表面活性剂P123作为模板剂,低相对分子质量酚醛树脂为碳源,正硅酸四乙酯为硅源,绿色无毒的表面活性剂Span80为扩孔剂,通过调整酚醛树脂及扩孔剂的用量,利用水热法制备出一系列功能性洋葱状介孔碳/硅复合材料。利用透射电子显微镜、扫描电子显微镜和氮气吸附-脱附等分析方法对洋葱状介孔碳/硅复合材料的颗粒形貌、粒径、比表面积、孔径分布进行表征,并研究了复合材料的吸附性能。结果表明,当扩孔剂Span80用量为0.4g,低相对分子质量酚醛树脂用量为1g、2g、3g时,合成的复合材料呈球形颗粒状,具有明显的层状结构,洋葱状形貌最佳,孔径在3～5nm之间,分布均一。洋葱状介孔碳/硅复合材料的氮气吸附-脱附等温线属于Ⅳ型等温线,滞后环为H2型滞后环,孔结构呈墨水瓶状。在最佳吸附条件下,洋葱状介孔碳/硅复合材料对罗丹明B和甲基橙染料的去除率均高达99%以上。
Nonionic surfactant P123 was used as the template agent,low molecular weight phenol-formaldehyde resin as the carbon source,tetraethyl orthosilicate as the silicon source,and green and nontoxic surfactant Span80 as reaming agent.A series of onion-like mesoporous carbon/silica materials were prepared by hydrothermal method and by adjusting the dosage of phenolic resin and reaming agent.The particle morphology,particle size,specific surface area and pore size distribution of the composites were characterized by transmission electron microscopy,scanning electron microscopy and nitrogen adsorption-desorption analysis,and the adsorption properties of the composites were studied.It was found that when the Span80 was 0.4g and the PF was 1g,2g,3g,the synthesized materials had an obvious lamellar structure and the onion shape was best.Spherical granules were spherical particles with pore size of 3～5nm and uniform distribution.Nitrogen adsorption desorption isotherm appeared as type Ⅳ isotherm,hysteresis loop was H2 hysteresis loop,and pore structure appeared hexagonal prism type.Under optimum adsorption conditions,the material removed Rhodamine B and methyl orange dyes was up to 99%.
[1] Forgacs E,Cserhati T,Oros G.Removal of synthetic dyes from wastewaters:a review[J].Environment International,2004,30(7):953-971.
[2] Gupta V K.Application of low-cost adsorbents for dye removal-a review[J].Journal of Environmental Management,2009,90(8):2313-2342.
[3] 刘友勋.染料的环境污染及其处理方法[J].中南论坛,2006,1(2):98-100;107.
[4] 蒋志国,王连军,于文敦.染料工业废水的治理方法[J].污染防治技术,2000,13(2):107-109.
[5] Tan I A W,Ahmad A L,Hameed B H.Adsorption of basic dye using activated carbon prepared from oil palm shell:batch and fixed bed studies[J].Desalination,2008,225(1/2/3):13-28.
[6] 徐文东,文湘华.微生物在含染料废水处理中的应用[J].环境污染治理技术与设备,2000,1(2):9-16.
[7] Engin A B,Özdemir Ö,Turan M,et al.Color removal from textile dyebath effluents in a zeolite fixed bed reactor:determination of optimum process conditions using Taguchi method[J].Journal of Hazardous Materials,2008,159(2):348-353.
[8] Avlonitis S A,Poulios I,Sotiriou D,et al.Simulated cotton dye effluents treatment and reuse by nanofiltration[J].Desalination,2008,221(1/2/3):259-267.
[9] Sun J,Hu Y,Bi Z,et al.Simultaneous decolorization of azo dye and bioelectricity generation using a microfiltration membrane air-cathode single-chamber microbial fuel cell[J].Bioresource Technology,2009,100(13):3185-3192.
[10] Rouquerol J,Avnir D,Fairbridge C W,et al.Recommendations for the characterization of porous solids[J].Pure and Applied Chemistry,1994,66(8):1739-1758.
[11] 陶大钧,张玮.大孔树脂吸附处理酚类胺类和其再生[J].化工环保,1990,10(5):267-271.
[12] 何炳林,黄文强.离子交换与吸附树脂[M].上海:上海科技教育出版社,1995:319-323.
[13] Vallet-Regi M,Rámila A,R P del Real,et al.A new property of MCM-41:drug delivery system[J].Chemistry of Materials,2001,2:308-311.
[14] Margolese D,Melero J A,Christiansen S C,et al.Direct syntheses of ordered SBA-15 mesoporous silica containing sulfonic acid groups[J].Chemistry of Materials,2000,12:2448-2459.
[15] Karkamkar A J,Kim S S,Mahanti S D,et al.Lamellar mesostructured silicas with chemically significant hierarchical morphologies[J].Advanced Functional Materials,2004,14(5):507-512.
[16] Tanev P T,Pinnavaia T J.Biomimetic templating of porous lamellar silicas by vesicular surfactant assemblies[J].Science,1996,271(5253):1267-1269.
[17] Zhang F,Meng Y,Gu D,et al.A facile aqueous route to synthesize highly ordered mesoporous polymers and carbon frameworks with Ia(3)over-bard bicontinuous cubic structure[J].Journal of the American Chemical Society,2005,127(39):13508-13509.
[18] Zhao D Y,Huo Q S,Feng J L,et al.Nonionic triblock and star diblock copolymer and oligomeric surfactant syntheses of highly ordered,hydrothermally stable,mesoporous silica structures[J].Journal of the American Chemical Society,1998,120(24):6024-6036.
[19] 陈精明,敖文亮,吴晓卫,等.甲阶酚醛树脂的合成研究进展[J].热固性树脂,2004,19(6):31-34.
[20] Yu Xianglin,Zhang Biyu,Rao Cong,et al.Effect of surfactants on the formation of onion-like mesoporous materials and their adsorption properties[J].Journal of Porous Maters,2016,23(4):1075-1083.
基金资助
国家自然科学基金(51203127);湖北省教育厅优秀中青年项目(20121509);武汉市科技局青年科技晨光计划项目(201050231049);绿色化工过程省部共建教育部重点实验室开放基金项目(GCP201003);武汉工程大学科学研究基金(10092012)
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