以设计合成的离子液体表面活性剂1-十六烷基-3-丙基咪唑溴盐为模板剂,正硅酸乙酯为硅源,通过水热合成法制备出了介孔MCM-41,结构表征表明其为孔道均一的六方有序结构,孔径3.28nm、比表面积967.08m2/g。研究了制备的MCM-41对有机染料亚甲基蓝的吸附性能,对此吸附过程进行了热力学和动力学分析。结果表明:当pH=9、吸附温度为35℃时吸附60min即达到吸附平衡,吸附量可达305.03mg/g。此吸附过程符合二级吸附动力学,属Freundlich等温吸附,吸附过程为吸热过程。
Mesoporous MCM-41 was prepared by hydrothermal synthesis method with self-designed and synthesized ironic liquid surfactant 1-hexadecyl-3-propylimidazolium bromide as templating agent and tetraethylorthosilicate as source of silicon.The structure characterization of the obtained MCM-41 indicated that the material possessed hexagonal pore structure with uniform channels,and its pore diameter and specific surface area were 3.24nm and 967.08m2/g,respectively.The adsorption properties of the prepared mesoporous MCM-41 for methylene blue were investigated,and the adsorption thermodynamics and kinetics were also analyzed.The results showed that the adsorption equilibrium was reached in 60 min under pH=9 and absorption temperature of 35℃,and the adsorption amount reached 305.03mg/g.The adsorption process belonged to Freundlich isothermal adsorption,conforming to the second-order adsorption kinetics,and the adsorption process was an endothermic process.
[1] Wang Y,Du X,Liu Z,et al.Dendritic fibrous nano-particles (DFNPs):rising stars of mesoporous materials[J].Journal of Materials Chemistry A,2019,7(10):5111-5152.
[2] Kumar M A,Krishn N V,Selvam P.Novel ionic liquid-templated ordered mesoporous aluminosilicates:synthesis,characterization and catalytic properties[J].Microporous and Mesoporous Materials,2019,275:172-179.
[3] Kresge C T,Leonowicz M E,Roth W J,et al.Ordered mesoporous molecular sieves synthesized by a liquid-crystal template mechanism[J].Nature,1992,359:710-712.
[4] 杨许召,白亚榕,张晨龙,等.哌啶类离子液体表面活性剂为模板制备介孔二氧化硅[J].轻工学报,2022,37(2):110-118.
[5] 喻娟.以离子液体为模板剂合成介孔分子筛MCM-41[D].郑州:郑州大学,2011.
[6] Trewyn B G,Whitman C M,Lin S Y.Morphological control of room-temperature ionic liquid templated mesoporous silica nanoparticles for controlled release of antibacterial agents[J].Nano Letters,2004,4(11):2139-2143.
[7] Wang J,Zhang C L,Bai Y R,et al.Synthesis of mesoporous silica with ionic liquid surfactant as template[J].Materials Letters,2021,291:129556.
[8] Yang Y,Deng C,Yuan Y Z.Characterization and hydroformylation performance of mesoporous MCM-41-supported water-soluble Rh complex dissolved in ionic liquids[J].Journal of Catalysis,2005,232(1):108-116.
[9] 孙振海,李滨,郭春垒,等.介孔氧化硅分子筛吸附性能研究进展[J].化工新型材料,2022,50(3):265-270.
[10] 李青翠,邓佑林,黄举朋.低成本制备MCM-41介孔分子筛及其对结晶紫的吸附性能[J].硅酸盐通报,2019,38(12):3807-3813,3821.
[11] 曾思思.粉煤灰合成Al-MCM-41及其吸附阳离子染料的吸附性能研究[D].沈阳:东北大学,2016.
[12] Sun T,Gong M F,Cai Y Q,et al.MCM-41-supported Fe(Mn)/Cu bimetallic heterogeneous catalysis for enhanced and recyclable photo-Fenton degradation of methylene blue[J].Research on Chemical Intermediates,2020,46(1):459-474.
[13] Yang X Z,Bai Y R,Li Q,et al.Preparation and adsorption properties of MCM-41 with novel Gemini ionic liquid surfactants as template[J].Materials,2022,15(8):2780.
[14] 安群力.介孔分子筛MCM-41的合成及性能研究[D].西安:西安科技大学,2005.
[15] Monash P,Pugazhenthi G.Investigation of equilibrium and kinetic parameters of methylene blue adsorption onto MCM-41[J].Korean Journal of Chemical Engineering,2010,27(4):1184-1191.
[16] 李娟娟,高歌.MCM-41介孔分子筛吸附性能的热力学和动力学分析[J].当代化工,2017,46(5):841-845.
[17] Ibrahim A A,Salama R S,El-Hakam S A,et al.Synthesis of sulfated zirconium supported MCM-41 composite with high-rate adsorption of methylene blue and excellent heterogeneous catalyst[J].Colloids and Surfaces A:Physicochemical & Engineering Aspects,2021,616:126361.
[18] Zhai Q Z.Studies of adsorption of crystal violet from aqueous solution by nano mesocellular foam (MCF) silica:process equilibrium,kinetic,isotherm,and thermodynamic studies[J].Water Science and Technology,2020,81(10):2092-2108.
[19] 魏健,宋永会,赵乐,等.Fenton氧化-序批式膜生物反应器耦合处理干法腈纶废水[J].环境工程学报,2013,7(6):2006-2012.
[20] 李薇,展侠,李继定,等.吸附氧化/纳滤/吸附组合工艺处理丙烯腈工业废水[J].环境工程学报,2013,7(4):1290-1294.
[21] 李勇.Fenton法处理腈纶废水技术研究[D].邯郸:河北工程大学,2010.
[22] 姜爽,吕琳琳,郭宏伟.榛子壳对亚甲基蓝吸附性能的研究[J].天然产物研究与开发,2017,29(1):110-113.
[23] 李云,袁志文.催化湿式氧化处理高浓度有机废水的研究进展[J].安徽农业科学,2013,41(13):5903-5905.
基金资助
河南省科技攻关项目(162102210056);郑州市科技攻关项目(141PQYJS555);郑州轻工业大学博士研究基金项目(2020BSJJ018)