Effect of Phosphoric Acid on HZSM-5 Catalysts for Prins Condensation to Isoprene from Isobutylene and Formaldehyde

doi:10.1007/s40242-018-7236-9

高等学校化学研究 ›› 2018, Vol. 34 ›› Issue (3): 485-489.doi: 10.1007/s40242-018-7236-9

Effect of Phosphoric Acid on HZSM-5 Catalysts for Prins Condensation to Isoprene from Isobutylene and Formaldehyde

YU Xue^1,2, ZHANG Yuewei², LIU Bing³, MA Huiyong⁴, WANG Yan⁵, BAO Qiang¹, WANG Zhenlü¹

1. Key Laboratory of Surface and Interface Chemistry of Jilin Province, College of Chemistry, Jilin University, Changchun 130021, P. R. China;
2. Jilin Institute of Chemical Technology, Jilin 132022, P. R. China;
3. State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, College of Chemistry, Jilin University, Changchun 130012, P. R. China;
4. Department of Medicinal Chemistry, University of Kansas, Kansas 66045, USA;
5. College of Chemistry and Biology of Beihua University, Jilin 132033, P. R. China

收稿日期:2017-07-11 修回日期:2018-01-03 出版日期:2018-06-01 发布日期:2018-05-24
通讯作者: WANG Zhenlü E-mail:wzl@jlu.edu.cn
基金资助:
Supported by the Jilin Province Science and Technology Research Plan(Key Scientific Research Project), China (No.20150204020GX), the Fund from the Technology Institute of Shanghai Huayi(Group) Company, China, the Open Subject of State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, China(No.2017-30) and the Youth Foundation of Jilin Province, China(No.20160520130JH).

Effect of Phosphoric Acid on HZSM-5 Catalysts for Prins Condensation to Isoprene from Isobutylene and Formaldehyde

YU Xue^1,2, ZHANG Yuewei², LIU Bing³, MA Huiyong⁴, WANG Yan⁵, BAO Qiang¹, WANG Zhenlü¹

1. Key Laboratory of Surface and Interface Chemistry of Jilin Province, College of Chemistry, Jilin University, Changchun 130021, P. R. China;
2. Jilin Institute of Chemical Technology, Jilin 132022, P. R. China;
3. State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, College of Chemistry, Jilin University, Changchun 130012, P. R. China;
4. Department of Medicinal Chemistry, University of Kansas, Kansas 66045, USA;
5. College of Chemistry and Biology of Beihua University, Jilin 132033, P. R. China

Received:2017-07-11 Revised:2018-01-03 Online:2018-06-01 Published:2018-05-24
Contact: WANG Zhenlü E-mail:wzl@jlu.edu.cn
Supported by:
Supported by the Jilin Province Science and Technology Research Plan(Key Scientific Research Project), China (No.20150204020GX), the Fund from the Technology Institute of Shanghai Huayi(Group) Company, China, the Open Subject of State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, China(No.2017-30) and the Youth Foundation of Jilin Province, China(No.20160520130JH).

摘要/Abstract

摘要： A series of HZSM-5 zeolites modified with different amounts of phosphoric acid(P/HZSM-5) was prepared. The physicochemical features of the P/HZSM-5 catalysts were characterized via X-ray diffraction(XRD), N₂ adsorption-desorption, NH₃-temperature programmed desorption(NH₃-TPD) and Fourier tranform infrared(FTIR) spectra of the adsorbed pyridine, and the performances of the catalysts for Prins condensation to isoprene from isobutylene and formaldehyde were investigated. The maximum isobutene conversion and isoprene selectivity were 10.3% and 94.6% on the HZSM-5 catalyst with a Si/Al molar ratio of 600 using 5%(mass fraction) phosphoric acid. The phosphoric acid modification not only modulated the amount of acidic sites but also regulated the acid type. An appropriate amount of weak Lewis and Brönsted acid sites served as the active sites for the condensation of isobutene with formaldehyde, and the strong acid sites could cause side reactions and coke deposition.

关键词: Isobutylene, Isoprene, Formaldehyde, HZSM-5 catalyst, Phosphoric acid modification

Abstract: A series of HZSM-5 zeolites modified with different amounts of phosphoric acid(P/HZSM-5) was prepared. The physicochemical features of the P/HZSM-5 catalysts were characterized via X-ray diffraction(XRD), N₂ adsorption-desorption, NH₃-temperature programmed desorption(NH₃-TPD) and Fourier tranform infrared(FTIR) spectra of the adsorbed pyridine, and the performances of the catalysts for Prins condensation to isoprene from isobutylene and formaldehyde were investigated. The maximum isobutene conversion and isoprene selectivity were 10.3% and 94.6% on the HZSM-5 catalyst with a Si/Al molar ratio of 600 using 5%(mass fraction) phosphoric acid. The phosphoric acid modification not only modulated the amount of acidic sites but also regulated the acid type. An appropriate amount of weak Lewis and Brönsted acid sites served as the active sites for the condensation of isobutene with formaldehyde, and the strong acid sites could cause side reactions and coke deposition.

Key words: Isobutylene, Isoprene, Formaldehyde, HZSM-5 catalyst, Phosphoric acid modification

YU Xue, ZHANG Yuewei, LIU Bing, MA Huiyong, WANG Yan, BAO Qiang, WANG Zhenlü. Effect of Phosphoric Acid on HZSM-5 Catalysts for Prins Condensation to Isoprene from Isobutylene and Formaldehyde[J]. 高等学校化学研究, 2018, 34(3): 485-489.

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Effect of Phosphoric Acid on HZSM-5 Catalysts for Prins Condensation to Isoprene from Isobutylene and Formaldehyde

Effect of Phosphoric Acid on HZSM-5 Catalysts for Prins Condensation to Isoprene from Isobutylene and Formaldehyde

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