Zr-SBA-15催化苯酚甲醛高选择性合成邻位异构体双酚F

doi:10.11949/j.issn.0438-1157.20151257

化工学报 ›› 2016, Vol. 67 ›› Issue (5): 1900-1906.DOI: 10.11949/j.issn.0438-1157.20151257

• 催化、动力学与反应器 • 上一篇下一篇

Zr-SBA-15催化苯酚甲醛高选择性合成邻位异构体双酚F

谈瑛, 李勇飞, 魏元峰, 严家其, 吴志民, 潘浪胜, 刘跃进

湘潭大学化工学院, 湖南湘潭 411105

收稿日期:2015-08-04 修回日期:2016-02-22 出版日期:2016-05-05 发布日期:2016-05-05
通讯作者: 刘跃进
基金资助:
国家自然科学基金项目(21276217)。

High selective synthesis of ortho isomer of bisphenol F catalyzed by Zr-SBA-15

TAN Ying, LI Yongfei, WEI Yuanfeng, YAN Jiaqi, WU Zhimin, PAN Langsheng, LIU Yuejin

College of Chemical Engineering, Xiangtan University, Xiangtan 411105, Hunan, China

Received:2015-08-04 Revised:2016-02-22 Online:2016-05-05 Published:2016-05-05
Supported by:
supported by the National Natural Science Foundation of China (21276217).

摘要/Abstract

摘要：

以P₁₂₃为模板剂,正硅酸乙酯为硅源,以硝酸氧锆为锆源,采用水热一步法合成了分子筛催化剂Zr-SBA-15,用XRD、BET、ICP、吡啶FT-IR、NH₃-TPD进行了分析表征,考察了不同Si/Zr摩尔比Zr-SBA-15催化苯酚、甲醛合成双酚F的催化活性,发现当Si/Zr摩尔比为20时催化活性较好。以Si/Zr摩尔比20的Zr-SBA-15为催化剂,在反应温度90℃、酚醛摩尔比30:1、催化剂与甲醛质量比1:1条件下反应240 min,双酚F收率达到83.5%,邻位异构体双酚F选择性高达92.5%,同时还提出了Zr-SBA-15高选择性催化苯酚、甲醛合成邻位异构体双酚F的反应机理。

关键词: 分子筛, 催化剂, 合成, 邻位异构体双酚F

Abstract:

A molecular sieve catalyst Zr-SBA-15 was synthesized by the hydrothermal one-step method using P₁₂₃, TEOS and ZrONO₃·xH₂O as template agent, silicon and zirconium sources, respectively. The Zr-SBA-15 catalyst was characterized by XRD, BET, ICP, pyridine-FTIR and NH₃-TPD, respectively, and used to mainly synthesize the ortho isomer of bisphenol F from phenol and formaldehyde. The results showed that the pore diameter of the prepared Zr-SBA-15 catalyst was about 6.6 nm and the distribution of pore diameter was uniform. After Zr incorporated into SBA-15, it had a high proportion of Lewis acid sites favouring the forming of the ortho isomer of bisphenol F with high catalytic activity. When the molar ratio of Si/Zr was 20, the Zr-SBA-15 catalyst exhibited the best catalytic activity with 83.5% of yield and 92.5% of ortho isomer of bisphenol F. The optimized reaction conditions were obtained as the phenol/formaldehyde molar ratio 30, the catalyst/formaldehyde mass ratio 1, reaction temperature 90℃ and reaction time 240 min. The reaction mechanism for high selective synthesis of the ortho isomer of bisphenol F was also proposed.

Key words: moleclar sieves, catalyst, synthesis, ortho isomer of bisphenol F

中图分类号:

谈瑛, 李勇飞, 魏元峰, 严家其, 吴志民, 潘浪胜, 刘跃进. Zr-SBA-15催化苯酚甲醛高选择性合成邻位异构体双酚F[J]. 化工学报, 2016, 67(5): 1900-1906.

TAN Ying, LI Yongfei, WEI Yuanfeng, YAN Jiaqi, WU Zhimin, PAN Langsheng, LIU Yuejin. High selective synthesis of ortho isomer of bisphenol F catalyzed by Zr-SBA-15[J]. CIESC Journal, 2016, 67(5): 1900-1906.

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Zr-SBA-15催化苯酚甲醛高选择性合成邻位异构体双酚F

High selective synthesis of ortho isomer of bisphenol F catalyzed by Zr-SBA-15

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