多级孔IM-5分子筛的简易制备及其在甲烷芳构化中的催化性能

LIU Heng; ZHOU Chen; ZHANG Yi-nan; KAN Qiu-bin

多级孔IM-5分子筛的简易制备及其在甲烷芳构化中的催化性能

刘恒^1, ,,
周晨¹,
张轶楠¹,
阚秋斌²

1.
长春理工大学纳米技术研究中心, 吉林长春 130022
2.
吉林大学化学学院, 吉林长春 130023

基金项目:

Youth Fund of Changchun University of Science and Technology XJJLG-2015-12

详细信息

中图分类号: O643
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- 被引次数: 0
出版历程
- 收稿日期: 2017-05-08
- 修回日期: 2017-07-19
- 网络出版日期: 2021-01-23
- 刊出日期: 2017-09-10

Facile preparation of hierarchically porous IM-5 zeolite with enhanced catalytic performance in methane aromatization

1.
Research Center for Nanotechnology, Changchun University of Science and Technology, Changchun 130022, China
2.
College of Chemistry, Jilin University, Changchun 130023, China

Funds:

Youth Fund of Changchun University of Science and Technology XJJLG-2015-12

More Information

Corresponding author: LIU Heng, k0431-85583121, E-mail:liuhengjlu@163.com

本文的英文电子版由 Elsevier 出版社在 ScienceDirect 上出版(http://www.sciencedirect.com/science/journal/18725813).

摘要

摘要: 采用一步水热晶化法、不添加第二模板剂、仅通过控制合成条件，制备了具有多级孔道结构的IM-5-H分子筛。多级孔IM-5-H材料展现了与常规IM-5-C分子筛不同的形貌、结构和酸性质。由于IM-5-H分子筛载体介孔结构的促进作用，钼基Mo-IM-5-H催化剂在甲烷无氧芳构化反应中表现出较高的甲烷转化率（13.1%）、芳烃产率（7.5%）和稳定性。该研究为合成多级孔IM-5材料提供了一种简便的方法，同时扩展了微孔-介孔复合材料在甲烷芳构化反应中的应用。
- 多级孔 /
- IM-5 /
- 沸石 /
- 甲烷芳构化
Abstract: A novel hierarchically porous IM-5-H zeolite material was prepared through one-step crystallization route by means of adjusting the synthesis parameters without introducing any secondary template.The hierarchical IM-5-H zeolite is quite different from the conventional IM-5-C in morphology, textural and acidic properties.After loading Mo, the Mo-IM-5-H catalyst exhibits high activity and stability in non-oxidative aromatization of methane, with a methane conversion of 13.1% and aromatics yield of 7.5%, owing to the mesopores in the IM-5-H zeolite crystals.This work provides a simple way to synthesize hierarchical IM-5 zeolite and expands the application of micro-mesoporous composite material in methane dehydroaromatization.
- hierarchical pore structure /
- IM-5 /
- zeolite /
- methane aromatization
本文的英文电子版由 Elsevier 出版社在 ScienceDirect 上出版(http://www.sciencedirect.com/science/journal/18725813).
注释:

HTML全文

Figure 1 XRD patterns of IM-5-H and IM-5-C samples

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Figure 2 SEM (a, b, c) and TEM (d, e, f) images of the IM-5-C (a, d) and IM-5-H (b, c, e, f) samples

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Figure 3 N₂ adsorption-desorption isotherms and pore size distributions of the IM-5-H(d, e, f) and IM-5-C(a, b, c) samples

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Figure 4 NH₃-TPD profiles of (a) H-IM-5-H, (b) Mo-IM-5-H, (c) H-IM-5-C, and (d) Mo-IM-5-C samples

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Figure 5 FT-IR spectra of pyridine adsorption on (a) H-IM-5-C, (b) Mo-IM-5-C, (c) H-IM-5-H, and (d) Mo-IM-5-H

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Figure 6 Performance of Mo-IM-5-H (●) and Mo-IM-5-C (■) catalysts in methane non-oxidative aromatization

reaction condition: 700℃, 1.01×10⁵Pa, and GHSV = 1500 h^-1

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Figure 7 Product selectivity for methane aromatization over Mo-IM-5-H and Mo-IM-5-C catalysts at 60 and 600min on stream

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Figure 8 TG curves of the spent Mo-IM-5-C and Mo-IM-5-H catalysts after methane aromatization tests

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Table 1 Surface areas (A_BET), microporous surface areas (v_micro), microporous volumes (v_micro), total pore volumes (v_total), micropore size (d_micro) and average pore size (d_aver) of the IM-5-C, Mo-IM-5-C, IM-5-H and Mo-IM-5-H samples

Sample	A_BET /(m²·g^-1)	A_micro /(m²·g^-1)	v_micro /(cm³·g^-1)	v_total /(cm³·g^-1)	d_micro /nm	d_aver /nm
IM-5-C	359	318	0.16	0.20	0.48	2.1
Mo-IM-5-C	302	274	0.14	0.17	0.45	1.9
IM-5-H	393	306	0.15	0.29	0.47	5.2
Mo-IM-5-H	321	265	0.13	0.24	0.45	4.7
note: d_micro is calculated from Horvath-Kawazoe report, whereas d_aver from BJH method based on the desorption branch

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Table 2 Acidity capacities of H-IM-5-C, Mo-IM-5-C, H-IM-5-H and Mo-IM-5-H

Sample	Peak area /(a.u.)
Sample	L	M	H
H-IM-5-C	466	-	570
Mo-IM-5-C	408	245	303
H-IM-5-H	395	-	397
Mo-IM-5-H	352	191	184

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Table 3 Quantitative results from pyridine-FT-IR spectra of H-IM-5-C, Mo-IM-5-C, H-IM-5-H and Mo-IM-5-H samples

Sample	Acidity quantity /(mmol·g^-1)
Sample	Brönsted acid sites	Lewis acid sites
H-IM-5-C	0.2723	0.2552
Mo-IM-5-C	0.2154	0.2179
H-IM-5-H	0.1917	0.2316
Mo-IM-5-H	0.1282	0.1975

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