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Study on pore regulation of high-silica MFI zeolites and their ethane/ethylene adsorption separation performances
- Low-carbon Chemistry and Chemical Engineering Vol. 49, Issue 11, Pages: 97-103(2024)
- 作者机构：
1.浙江工业大学 化学工程学院 催化反应工程研究所，浙江 杭州 310014
2.浙江环境科技有限公司，浙江 杭州 311121
- 作者简介：
- 基金信息：
DOI：10.12434/j.issn.2097-2547.20240243
CLC： TQ424.23Published：25 November 2024，
Received：01 June 2024，
Revised：15 July 2024，
- 稿件说明：
移动端阅览
熊峰,柯权力,卢梅等.高硅MFI分子筛孔道调控及其乙烷/乙烯吸附分离性能研究[J].低碳化学与化工,2024,49(11):97-103.
XIONG Feng,KE Quanli,LU Mei,et al.Study on pore regulation of high-silica MFI zeolites and their ethane/ethylene adsorption separation performances[J].Low-carbon Chemistry and Chemical Engineering,2024,49(11):97-103.
熊峰,柯权力,卢梅等.高硅MFI分子筛孔道调控及其乙烷/乙烯吸附分离性能研究[J].低碳化学与化工,2024,49(11):97-103. DOI： 10.12434/j.issn.2097-2547.20240243.
XIONG Feng,KE Quanli,LU Mei,et al.Study on pore regulation of high-silica MFI zeolites and their ethane/ethylene adsorption separation performances[J].Low-carbon Chemistry and Chemical Engineering,2024,49(11):97-103. DOI： 10.12434/j.issn.2097-2547.20240243.
摘要
借助固体吸附分离技术可获得高纯度乙烯，对提高乙烯产品质量有重要意义。采用表面修饰策略对Mn掺杂高硅MFI分子筛（H-MFI-Mn）进行修饰分别制得P修饰H-MFI-Mn（H-MFI-Mn-P）和HCOOH修饰H-MFI-Mn（H-MFI-Mn-COOH和H-MFI-Mn-P-COOH）。采用XRD、SEM和N
2
吸/脱附等对所得分子筛进行了表征。在混合气体中（
V
(乙烯):
V
(乙烷) = 50:50）对所得分子筛的乙烷/乙烯吸附分离性能进行了评价，并采用UV-Vis和XPS对所得分子筛的乙烷/乙烯吸附分离机理进行了分析。结果表明，H-MFI-Mn-P-COOH的微孔孔径（0.68 nm）和平均孔径（2.70 nm）较H-MFI-Mn的孔径（0.55 nm）和平均孔径（1.61 nm）明显增大。与H-MFI-Mn的比表面积（446 m
2
/g）相比，H-MFI-Mn-P、H-MFI-Mn-COOH和H-MFI-Mn-P-COOH的比表面积（400 m
2
/g左右）均有所减小。H-MFI-Mn-P-COOH表现出较好的乙烷/乙烯吸附分离性能，其乙烷动态平衡吸附容量为1 mmol/g，乙烷/乙烯动态分离选择性为2.08。与H-MFI-Mn相比，H-MFI-Mn-P-COOH中Mn
3+
和Mn
2+
在总Mn离子中的占比较高，说明P修饰+ HCOOH修饰可削弱分子筛结构中Mn
δ
+
物种的电子转移性能，进而抑制H-MFI-Mn-P-COOH的乙烯吸附性能。
Abstract
High purity ethylene can be obtained by the solid adsorption separation technology
which is of great significance to improve the quality of ethylene products. Mn-doped high-silica MFI zeolite (H-MFI-Mn) were modified by surface modification strategy to obtain P-modified H-MFI-Mn (H-MFI-Mn-P) and HCOOH-modified H-MFI-Mn (H-MFI-Mn-COOH and H-MFI-Mn-P-COOH)
respectively. The prepared zeolites were characterized by XRD
SEM and N
2
adsorption/desorption
etc. The ethane/ethylene adsorption separation performances of prepar
ed zeolites were evaluated in mixed gas (
V
(ethane):
V
(ethylene) = 50:50). And the ethane/ethylene adsorption separation mechanisms of prepared zeolites were analyzed by UV-Vis and XPS. The results show that the micropore size (0.68 nm) and average pore size (2.70 nm) of H-MFI-Mn-P-COOH are significantly larger than the micropore size (0.55 nm) and average pore size (1.61 nm) of H-MFI-Mn. Compared with the specific surface area of H-MFI-Mn (446 m
2
/g)
the specific surface areas (about 400 m
2
/g) of H-MFI-Mn-P
H-MFI-Mn-COOH and H-MFI-Mn-P-COOH decrease. H-MFI-Mn-P-COOH shows better ethane/ethylene adsorption separation performance with ethane dynamic equilibrium adsorption capacity of 1 mmol/g and ethane/ethylene dynamic separation selectivity of 2.08. Compared with H-MFI-Mn
Mn
3+
and Mn
2+
in H-MFI-Mn-P-COOH accounted for higher proportions in total Mn ions
indicating that P-modification + HCOOH-modification can weaken the electron transfer performance of Mn
δ
+
species in the zeolite structure
and then inhibit the ethylene adsorption performance of H-MFI-Mn-P-COOH.
关键词
高硅MFI分子筛乙烷/乙烯吸附分离表面修饰
Keywords
high-silica MFI zeolitesethane/ethylene adsorption separationsurface modification
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