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低模板剂用量下Silicalite-1分子筛中介孔结构的调控及甲醇制丙烯反应性能研究
Study on regulation of mesoporous structures of Silicalite-1 molecular sieves under low template dosage and reaction performances in methanol to propene
- 低碳化学与化工 2024, 49(10): 20-29.
- 作者机构：
1.重庆科技大学 化学化工学院，重庆 401331
2.重庆市计量质量检测研究院，重庆 401331
- 作者简介：
孟晓静（1987—），博士，讲师，研究方向为甲醇制烯烃催化剂制备及工艺开发，E-mail：mengxiaojing88@126.com。
- 基金信息：国家自然科学基金(22202026)
DOI：10.12434/j.issn.2097-2547.20230393
中图分类号： TQ032;O643.36纸质出版日期：2024-10-25，
收稿日期：2023-11-29，
修回日期：2023-12-29，
- 稿件说明：
移动端阅览
孟晓静,张阳,孟晓伟等.低模板剂用量下Silicalite-1分子筛中介孔结构的调控及甲醇制丙烯反应性能研究[J].低碳化学与化工,2024,49(10):20-29.
MENG Xiaojing,ZHANG Yang,MENG Xiaowei,et al.Study on regulation of mesoporous structures of Silicalite-1 molecular sieves under low template dosage and reaction performances in methanol to propene[J].Low-carbon Chemistry and Chemical Engineering,2024,49(10):20-29.
孟晓静,张阳,孟晓伟等.低模板剂用量下Silicalite-1分子筛中介孔结构的调控及甲醇制丙烯反应性能研究[J].低碳化学与化工,2024,49(10):20-29. DOI： 10.12434/j.issn.2097-2547.20230393.
MENG Xiaojing,ZHANG Yang,MENG Xiaowei,et al.Study on regulation of mesoporous structures of Silicalite-1 molecular sieves under low template dosage and reaction performances in methanol to propene[J].Low-carbon Chemistry and Chemical Engineering,2024,49(10):20-29. DOI： 10.12434/j.issn.2097-2547.20230393.
摘要
针对微孔Silicalite-1分子筛扩散阻力和合成成本高的问题，采用晶种诱导法在低模板剂用量（
n
(TPA
+
):
n
(Si) = 0.01，TPA
+
为四丙基铵离子）下合成了多级孔Silicalite-1分子筛。采用XRD、FT-IR和N
2
吸/脱附等对分子筛进行了表征并研究了其在甲醇制丙烯反应中的催化性能。结果表明，对于一段晶化制备的分子筛，当晶种在合成凝胶中的质量分数为10%，氟化钠与Si的物质的量之比为0.8时所得分子筛（S-1
10
-0.01-NH
4
F
0.8
）具有较理想的结构，其介孔孔容为0.120 cm
3
/g。对于两段晶化制备的分子筛，当低温段晶化时间为6 h，晶种在合成凝胶中的质量分数为10%，尿素与Si的物质的量之比为0.5时所得分子筛（SL-1
10
-0.01-6-CH
4
N
2
O
0.5
）具有较理想的结构，其介孔孔容为0.220 cm
3
/g。在450 ℃、甲醇质量空速为5.53 h
-1
的条件下反应30~40 min，SL-1
10
-0.01-6-CH
4
N
2
O
0.5
表现出相对较好的催化性能，其丙烯产率为14.65%，
m
(丙烯):
m
(乙烯)为4.6，再生周期为2600 min。
Abstract
In order to solve the problems of high diffusion resistance and high synthesis cost of microporous Silicalite-1 molecular sieves
hierarchical Silicalite-1 molecular sieves were synthesized by seed induction method under low dosage of template agent (
n
(TPA
+
):
n
(Si) = 0.01
TPA
+
is tetrapropylammonium ion). The molecular sieves were characterized by XRD
FT-IR and N
2
adsorption/desorption
and their catalytic performances in methanol to propylene were studied. The results show that for the molecular sieves prepared by one stage crystallization
when the mass fraction of seed in synthesized gel is 10% and the molar ratio of sodium fluoride to Si is 0.8
the obtained molecular sieve (S-1
10
-0.01-NH
4
F
0.8
) has an ideal structure
and its mesoporous pore capacity is 0.120 cm
3
/g. For the molecular sieve prepared by two-stage crystallization
when the crystallization time of the low-temperature phase is 6 h
the mass fraction of seed in synthesized gel is 10%
the molar ratio of urea to Si is 0.5
the obtained molecular sieve (SL-1
10
-0.01-6-CH
4
N
2
O
0.5
) has an ideal structure
and its mesoporous pore capacity is 0.220 cm
3
/g. Under the re
action conditions of 450 ℃ and methanol mass space velocity of 5.53 h
-1
for 30 min to 40 min
SL-110-0.01-6-CH
4
N
2
O
0.5
exhibits relatively good catalytic performance with the propylene yield of 14.65%
m
(propylene):
m
(ethylene) of 4.6 and the regeneration period of 2600 min.
关键词
多级孔Silicalite-1分子筛晶种甲醇制丙烯
Keywords
hierarchical Silicalite-1 molecular sievesseedmethanol to propene
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