介孔分子筛KF-SBA-15的制备及其催化Knoevenagel反应

摘要以P123、正硅酸四乙酯、KF为原料制备了介孔分子筛SBA-15及KF-SBA-15，使用XRD、IR、BET和TG等确证结构。在以苯甲醛和丙二腈为探针的Knoevenagel缩合反应中考察其催化性能，单因素实验法优化反应条件，探究催化剂类型及用量、溶剂、原料物质的量之比等对产率的影响，筛选出最适宜条件为：n（苯甲醛）：n（丙二腈）为1：1，催化剂用量为醛的10%（摩尔分数，下同），室温反应30 min产率可达93.6%。

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	李琳琳
	龚维
	付海
	裴响林
	陈卓
	尹晓刚

关键词： Knoevenagel反应 SBA-15 KF 负载型催化剂

Abstract： Mesoporous molecular sieves SBA-15 and KF-SBA-15, were prepared by using P123 tetraethyl orthosilicate and KF as raw materials, and the structures were confirmed by IR, BET, TG and XRD. The Knoevenagel condensation reaction of benzaldehyde and malononitrile was catalyzed by mesoporous molecular sieve KF-SBA-15. The effects of catalyst dosage, solvent, molar ratio of raw materials and catalyst type on the yield were investigated. The optimum conditions were as follows: the ratio of aromatic aldehyde to malononitrile was 1:1, the amount of catalyst was 10%(mole fraction) of benzaldehyde. The reaction was carried out for 30 min at room temperature and the yields could be 93.6%.

Keywords： Knoevenagel reaction； SBA-15； KF； supported catalyst

Received 2019-04-15;

Fund:贵州省科技创新人才团队建设项目（黔科合人才团队[2014]4006号）。

Corresponding Authors: 尹晓刚,E-mail:m13885115516@163.com。 Email: m13885115516@163.com

About author: 李琳琳(1990-),女,硕士研究生,主要从事有机合成研究。

引用本文:

李琳琳, 龚维, 付海, 裴响林, 陈卓, 尹晓刚.介孔分子筛KF-SBA-15的制备及其催化Knoevenagel反应[J]. 化学工业与工程, 2020,37(3): 17-22

Li Linlin, Gong Wei, Fu Hai, Pei Xianglin, Chen Zhuo, Yin Xiaogang.Preparation of KF-SBA-15 and its Catalytic Knoevenagel Reaction[J]. Chemcial Industry and Engineering, 2020,37(3): 17-22

[1] 刘雄伟, 姜恒, 宫红. 室温无溶剂条件下醋酸锌催化的Knoevenagel缩合反应[J]. 有机化学, 2007, 27(1):131-133 Liu Xiongwei, Jiang Heng, Gong Hong. Knoevenagel condensation catalyzed by zinc acetate under solvent free condition at room temperature[J]. Chinese Journal of Organic Chemistry, 2007, 27(1):131-133(in Chinese)
[2] 薛冰, 刘香梅, 柳娜, 等. 氨水改性氧化石墨烯高效催化Knoevenagel缩合反应[J]. 精细化工, 2017, 5(9):1-11 Xue Bing, Liu Xiangmei, Liu Na, et al. Ammonia modified graphene oxide catalyzed Knoevenagel condensation[J]. Fine Chemical Industry, 2017, 5(9):1-11(in Chinese)
[3] 张艳梅, 戴田霖, 张帆, 等. 核壳结构Fe₃O₄@UiO-66-NH₂磁性纳米复合材料的合成及其催化Knoevenagel缩合反应性能[J]. 催化学报, 2016, 37(12):2106-2113 Zhang Yanmei, Dai Tianlin, Zhang Fan, et al. Fe₃O₄@UiO-66-NH₂ core-shell nanohybrid as stable heterogeneous catalyst for Knoevenagel condensation[J]. Chinese Journal of Catalysis, 2016, 37(12):2106-2113
[4] 孙锦玉, 赵东元. "面包圈"状高有序度大孔径介孔分子筛SBA-15的合成[J]. 高等学校化学学报, 2000, 21(1):21-23 Sun Jinyu, Zhao Dongyuan. Synthesis of highly ordered donut-like mesoporous silica SBA-15[J]. Chemical Research in Chinese Universities, 2000, 21(1):21-23(in Chinese)
[5] Lin H, Zheng J, Zheng X, et al. Improved chemoselective hydrogenation of crotonaldehyde over bimetallic AuAg/SBA-15 catalyst[J]. Journal of Catalysis, 2015, 330:135-144
[6] Cotea V V, Luchian C E, Bilba N, et al. Mesoporous silica SBA-15, a new adsorbent for bioactive polyphenols from red wine[J]. Analytica Chimica Acta, 2012, 732:180-185
[7] Fathi V V, Mohammadi Z G, Badiei A. The role of SBA-15 in drug delivery[J]. RSC Advances, 2015, 5(111):91686-91707
[8] Ngene P, Adelhelm P, Beale A M, et al. LiBH₄/SBA-15 nanocomposites prepared by melt infiltration under hydrogen pressure:Synthesis and hydrogen sorption properties[J]. The Journal of Physical Chemistry C, 2010, 114(13):6163-6168
[9] 张雪峥, 乐英红, 高滋. SBA-15负载氧化铁催化剂上乙酸选择加氢制乙醛[J]. 高等学校化学学报, 2003, 24(1):121-124 Zhang Xuezheng, Yue Yinghong, Gao Zi. Selective hydrogenation of acetic acid to acetaldehyde over SBA-15 supported iron oxide catalysts[J]. Chemical Research in Chinese Universities, 2003, 24(1):121-124(in Chinese)
[10] 张飞豹, 张蔡华, 邓元, 等. SBA-15负载Pd催化剂的制备及其在Heck反应中的应用研究[J]. 化学学报, 2010, 68(5):443-448 Zhang Feibao, Zhang Caihua, Deng Yuan, et al. Palladium supported on SBA-15 as a new recyclable catalyst for the mizoroki-heck reaction[J]. Acta Chimica Sinica, 2010, 68(5):443-448(in Chinese)
[11] 岳彩波, 魏运洋. 功能性离子液体催化Knoevenagel缩合反应[J]. 精细化工, 2007, 24(2):166-168 Yue Caibo, Wei Yunyang. Knoevenagel condensation reaction catalyzed by task specific ionic liquid[J]. Fine Chemicals, 2007, 24(2):166-168(in Chinese)
[12] 隆金桥, 罗志荣, 苏丽清, 等. 分子筛SBA-15负载磷钨酸催化合成苯甲醛乙二醇缩醛[J]. 中国钨业, 2015, 10(3):58-62 Long Jinqiao, Luo Zhirong, Su Liqing, et al. Synthesis of benzaldehyde glycol acetal catalyzed by phosphotungstic acid supported on SBA-15 molecular sieve[J]. China Tungsten Industry, 2015, 10(3):58-62(in Chinese)
[13] 袁兴东, 沈健, 李国辉, 等. 表面含磺酸基的介孔分子筛SBA-15-SO₃H的直接合成[J]. 催化学报, 2003, 24(2):83-86 Yuan Xingdong, Shen Jian, Li Guohui, et al. Direct synthesis of SBA-15 mesoporous silica functionalized with sulfonic acid groups[J]. Chinese Journal of Catalysis, 2003, 24(2):83-86(in Chinese)
[14] Ren Z, Cao W, Tong W. The Knoevenagel condensation reaction of aromatic aldehydes with malononitrile by grinding in the absence of solvents and catalysts[J]. Chem Inform, 2003, doi:10.1002/chin.200310091
[15] Colilla M, Izquierdo-Barba I, Sänchez-Salcedo S, et al. Synthesis and characterization of zwitterionic SBA-15 nanostructured materials[J]. Chemistry of Materials, 2010, 22(23):6459-6466
[16] Garcia-Cuello V S, Giraldo L, Moreno-Pirajän J C. Synthesis, characterization, and application in the CO oxidation over a copper nanocatalyst confined in SBA-15[J]. Journal of Chemical & Engineering Data, 2011, 56(4):1167-1173