[1]李建祥,张需鹏,康豪,等.甲醛与乙烯Prins缩合反应固体酸催化剂的制备与性能评价[J].石化技术与应用,2023,6:428-432.
LI Jian-xiang,ZHANG Xu-peng,KANG Hao,et al.Preparation and performance evaluation of solid acid catalyst for Prins condensation of formaldehyde and ethylene[J].Petrochemical technology & application,2023,6:428-432.
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甲醛与乙烯Prins缩合反应固体酸催化剂的制备与性能评价(PDF)
《石化技术与应用》[ISSN:1009-0046/CN:62-1138/TQ]
- 期数:
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2023年6期
- 页码:
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428-432
- 栏目:
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- 出版日期:
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2023-11-10
文章信息/Info
- Title:
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Preparation and performance evaluation of solid acid catalyst for Prins condensation of formaldehyde and ethylene
- 文章编号:
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1009-0045(2023)06-0428-05
- 作者:
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李建祥1; 张需鹏2; 康豪1; 张强1*
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1.中国石油大学(华东) 化学化工学院 重质油国家重点实验室,山东 青岛 266500;2.胜华新材料股份有限公司,山东 东营 257041
- Author(s):
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LI Jian-xiang1; ZHANG Xu-peng2; KANG Hao1; ZHANG Qiang1
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1.State Key Laboratory of Heavy Oil Processing,College of Chemistry and Chemical Engineering,China University of Petroleum(East China),Qingdao 266500,China;2.Shenghua New Materials Co Ltd,Dongying 257041, China
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- 关键词:
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甲醛; 乙烯; 对甲苯磺酸; Prins反应; 硅基载体; 固体酸
- Keywords:
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formaldehyde; ethylene; p-toluene sulfonic acid; Prins reaction; silicon-based carrier; solid acid
- 分类号:
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TQ 426.94
- DOI:
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DOI:10.19909/j.cnki.ISSN1009-0045.2023.06.0428
- 文献标识码:
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B
- 摘要:
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采用浸渍法将对甲苯磺酸(p-TSA)负载到4种不同硅基载体(SiO2,SiO2-La2O3,SBA-15和Silicalite)上制备了相应的固体酸催化剂,利用X射线衍射仪、物理吸附仪、傅立叶变换红外光谱仪、元素分析等表征手段对系列催化剂进行了表征;并与液体酸催化剂p-TSA相比较,以甲醛与乙烯的Prins反应,考察了载体对固体酸催化剂催化性能的影响。结果表明:硅基载体的比表面积和孔径越大,越有利于p-TSA分散;p-TSA在SiO2和SBA-15表面分散更均匀;以SiO2为载体所得固体酸催化剂的B酸酸量较高;在p-TSA用量相当的情况下,固体酸催化剂的催化性能均优于液体酸催化剂p-TSA的;在p-TSA负载量为55%时,以SiO2为载体所得固体酸p-TSA/SiO2作催化剂时,甲醛转化率以及1, 3-二氧六环收率和选择性均最佳,依次为87.73%,20.81%和23.73%。
- Abstract:
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The corresponding solid acid catalyst was prepared by impregnating p-toluene sulfonic acid (p-TSA) onto 4 different silicon-based carriers (SiO2,SiO2-La2O3,SBA-15 and Silicalite). The catalysts were characterized by methods of X-ray diffraction, physical adsorption,Fourier transform infrared spectrometer and elemental analysis. Comparing with the liquid acid p-TSA catalyst,the effect of the support on the catalytic performance of solid acid catalyst was investigated by Prins reaction of formaldehyde and ethylene. The results showed that the larger specific surface area and pore size of silicon-based carrier,the better dispersion of p-TSA. p-TSA was more evenly dispersed on SiO2 and SBA-15 surfaces. The B acid content of solid acid catalyst obtained with SiO2 as the carrier was higher. The catalytic performance of solid acid catalyst was better than that of liquid acid p-TSA catalyst when the amount of p-TSA was the same. When the loading of p-TSA was at 55% and the solid acid p-TSA/SiO2 with SiO2 as the carrier was used as the catalyst,the formaldehyde conversion rate,1,3-dioxanocyclic yield and selectivity were the best,which were 87.73%,20.81% and 23.73%,respectively.
参考文献/References
[1] Wang Y H,Zhang J,Zhang Z X,et al. The in situ transformation of the co-product formaldehyde in the reversible hydrolysis of 1,3-dixoane to obtain 1,3-propanediol efficiently[J]. Green Chemistry,2018,20(7):1455-1458.[2] Fabio M,Guido P,Stefano Z. The reactivity of molybdenum pentachloride with ethers: Routes to the synthesis of Mo(Ⅳ)Cl4 adducts,Mo(Ⅴ) chlorido-alkoxides and Mo(Ⅴ) oxydo-chlorides[J]. Dalton Transactions,2013, 42(42):15226-15234.[3] Medina F,Besnard C,Lacour J. One-step synthesis of nitrogen-containing medium-sized rings via α-imino diazo intermediates[J]. Organic Letters,2014,16(12):3232-3235.[4] Hellmuth M,Chen B J,Bariki C,et al. A comparative study on the combustion chemistry of two bio-hybrid fuels: 1,3-dioxane and 1,3-dioxolane[J]. The Journal of Physical Chemistry(A), 2023,127(1):286-299.[5] 于政锡,张英伟,许磊,等. 一种1,3-二噁烷的制备方法:中国,103130767 A[P]. 2013-06-05.[6] 薛丽梅, 王琲, 韩大维,等. 1,3-丙二醇的化学合成法[J]. 化学与粘合,2000(1): 38-40.[7] Adelman D J,Drysdale N E. Manufacture of 1,3-propanediol esters from formaldehyde and ethylene using a modified Prins reaction: US,6111135[P]. 2000-08-29.[8] 王峰,王业红,徐杰,等. 一种由烯烃直接制备1,3-二元醇的方法:中国,103102229 A[P]. 2013-05-15.[9] 王泽宇,李学坤,雄赳赳,等. 碳基固体磺酸催化剂制备及应用[J]. 山东化工,2021,50(4): 10-11.[10] 韩振. 高效磺酸型固体酸的研究[D]. 上海: 华东师范大学,2016.
备注/Memo
- 备注/Memo:
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山东省重点研发计划(重大科技创新工程)资助项目(项目编号:2021 ZLGX 06)
更新日期/Last Update:
2023-11-10