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投稿时间：2018-08-24 修订日期：2018-10-18
投稿时间：2018-08-24 修订日期：2018-10-18
中文摘要: 首先通过4-硝基邻苯二腈分别与对羟基苯甲酸和N,N-二甲基乙醇胺反应制备了4-（4-羧基苯氧基）邻苯二腈（CPPN）和4-(N,N-二甲胺基乙氧基)邻苯二腈(ePN)，然后利用开环反应将CPPN键合到聚甲基丙烯酸缩水甘油酯改性的硅胶（PGMA/SiO2）表面，得到键合有邻苯二腈的硅胶CPPN-PGMA/SiO2。最后，在“分子碎片”ePN和催化剂DBU作用下，通过“同步合成与固载”的方法在PGMA/SiO2表面固载金属酞菁（β-(N,N-二甲胺基乙氧基)酞菁锌，ePcZn）或无金属酞菁（ePc），从而制备了固载化的酞菁ePcZn-PGMA/SiO2或ePc-PGMA/SiO2。通过FT-IR、紫外-可见光谱、TGA等对其结构和酞菁键合量进行表征和测定。考察了DBU的用量对“同步合成与固载”酞菁过程的影响。最后以亚甲基蓝(MB)为目标降解物，研究所制得的固载化酞菁催化剂ePc-PGMA/SiO2或ePcZn-PGMA/SiO2的可见光催化活性。结果表明，借助“同步合成与固载”的方法能够成功在PGMA/SiO2表面固载ePc或ePcZn，得到固载化酞菁光催化剂ePc-PGMA/SiO2或ePcZn-PGMA/SiO2，它们均具有较好的可见光催化活性。在可见光照射下，ePcZn-PGMA/SiO2和ePc-PGMA/SiO2在较低的浓度下 (0.2 g/L)凭借吸附-光催化耦合协同作用均能有效降解MB，且随催化剂浓度的增大，MB的降解率增大，0.6 g/L的ePcZn-PGMA/SiO2能使MB的降解率高达92 % 以上。催化剂重复4次后仍具有较好的光催化稳定性。
中文关键词: β-(N,N-二甲胺基乙氧基)酞菁 同步合成 固载 硅胶 聚甲基丙烯酸缩水甘油酯 光催化活性
Abstract:4-(4-carboxyl group)-O-benzene phthalonitrile (CPPN) and 4-(N,N-dimethylaminoethoxy) phthalonitrile (ePN) were first prepared by reacting 4-nitrophthalonitrile with p-hydroxybenzoic acid and N,N-dimethylethanolamine, respectively. Then, the silica gel bonded with phthalonitrile CPPN-PGMA/SiO2 was obtained by means of the ring opening reaction between CPPN and polyglycidyl methacrylate-modified silica (PGMA/SiO2). Finally, under the action of “molecular fragment” ePN and catalyst DBU, β-(N,N-dimethylaminoethoxy) zinc phthalocyanine (ePcZn) and metal-free phthalocyanine (ePc) was supported on the surface of PGMA/SiO2 by the method of “synchronous synthesis and immobilization” to prepare the immobilized phthalocyanine ePc-PGMA/SiO2 or ePcZn-PGMA/SiO2. of them were characterized by FT-IR, and TG. And their UV-visible spectra were determined. Their structures and phthalocyanine binding amounts were characterized by FT-IR and UV-Vis diffuse reflectance spectroscopy, and phthalocyanine binding amounts were determined by TG. The effect of the dosage of DBU on the immobilized reaction of phthalocyanine was investigated. In addition, with the organic dye methylene blue (MB) as the target degradation material, the photocatalytic properties of immobilized phthalocyanine catalyst ePc-PGMA/SiO2 and ePcZn-PGMA/SiO2 were researched. The results showed that phthalocyanine could be immobilized onto PGMA/SiO2 successfully by the method of synchronous synthesis and immobilization, obtaining the immobilized photocatalyst ePc-PGMA/SiO2 and ePcZn-PGMA/SiO2. The prepared ePcZn-PGMA/SiO2 and ePc-PGMA/SiO2 both have the good photocatalytic activity. ePcZn-PGMA/SiO2 and ePc-PGMA/SiO2 can effectively catalyze the degradation of MB by adsorption and photocatalysis at the lower concentration (0.2 g / L) under visible light irradiation. The degradation rate of MB increases with the increasing concentration of ePcZn-PGMA/SiO2, and the degradation rate of MB is over than 92 % with 0.6 g/L ePcZn-PGMA/SiO2. Moreover, the ePcZn-PGMA/SiO2 showed reliable photocatalytic activity after four times reuse．
keywords: β-(N,N-dimethylaminoethoxy) phthalocyanine zinc synchronous synthesis immobilization silica gel polyglycidyl methacrylate photocatalytic activity
文章编号：20180824001 中图分类号：O69 文献标志码：
基金项目:中北大学超重力化工过程重点实验室开放基金( CZL201506) 资助；山西省高等学校优秀青年术带头人支持计划( 201510)
| Author Name | Affiliation | Postcode |
| DANG Lifang | North University of China | |
| LIU Yefeng | North University of China | |
| ZHANG Rongrong | North University of China | |
| JIAO Weizhou | North University of China | |
| WANG Ruixin | North University of China | 030051 |
引用本文：
党利芳,刘叶峰,张荣荣,焦纬洲,王蕊欣.β-(N,N-二甲胺基乙氧基)酞菁锌的同步合成与固载及其光催化活性[J].功能高分子学报,DOI:10.14133/j.cnki.1008-9357.20180824001.
DANG Lifang,LIU Yefeng,ZHANG Rongrong,JIAO Weizhou,WANG Ruixin.Synchronous Synthesis and Immobilization of β-(N,N-dimethylaminoethoxy) Phthalocyanine Zinc on Silica Surface and Its Photocatalytic Activity[J].Journal of Functional Polymers,DOI:10.14133/j.cnki.1008-9357.20180824001.
党利芳,刘叶峰,张荣荣,焦纬洲,王蕊欣.β-(N,N-二甲胺基乙氧基)酞菁锌的同步合成与固载及其光催化活性[J].功能高分子学报,DOI:10.14133/j.cnki.1008-9357.20180824001.
DANG Lifang,LIU Yefeng,ZHANG Rongrong,JIAO Weizhou,WANG Ruixin.Synchronous Synthesis and Immobilization of β-(N,N-dimethylaminoethoxy) Phthalocyanine Zinc on Silica Surface and Its Photocatalytic Activity[J].Journal of Functional Polymers,DOI:10.14133/j.cnki.1008-9357.20180824001.
