孪晶HZSM-5@Silicalite-1核壳结构催化剂的制备及甲苯甲醇烷基化性能研究

潘旭; 杜冰; 黄鑫; 王瑞壮; 韦慧; 张海永; 刘意; 许德平

doi:10.19906/j.cnki.JFCT.2021095

孪晶HZSM-5@Silicalite-1核壳结构催化剂的制备及甲苯甲醇烷基化性能研究

doi: 10.19906/j.cnki.JFCT.2021095

潘旭¹,
杜冰^2, ,,
黄鑫²,
王瑞壮²,
韦慧²,
张海永¹,
刘意^2, ,,
许德平¹

1.
中国矿业大学(北京) 化学与环境工程学院, 北京 100083
2.
北京低碳清洁能源研究院, 北京 102209

详细信息

通讯作者:
E-mail: 17240143@chnenergy.com.cn

yi.liu.ft@chnenergy.com.cn

中图分类号: O643
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- 被引次数: 0
出版历程
- 收稿日期: 2021-10-28
- 修回日期: 2021-12-06
- 录用日期: 2021-12-06
- 网络出版日期: 2021-12-20
- 刊出日期: 2022-05-24

Preparation of core-shell structural twin HZSM-5@Silicalite-1 catalysts and its performance for toluene alkylation with methanol

1.
China University of Mining and Technology-Beijing, School of Chemical & Environmental Engineering, Beijing 100083, China
2.
National Institute of Clear-and-Low-Carbon Energy, Beijing 102209, China

摘要

摘要: 本研究采用水热结晶法合成了孪晶HZSM-5分子筛，并在表面外延生长Silicalite-1（S-1）纯硅沸石，制备了HZSM-5@Silicalite-1核壳结构催化剂。与孪晶HZSM-5相比，HZSM-5@Silicalite-1核壳结构催化剂在甲苯甲醇烷基化反应中表现出优异的催化性能。在470 ℃、0.1 MPa和临氢反应条件下，HZSM-5@40Silicalite-1催化剂的甲苯单程转化率为8.5%，对二甲苯选择性为98.4%。进一步研究了核相HZSM-5与S-1壳层前驱体固液质量比对表面S-1晶体生长的影响，同时考察了S-1壳层对孪晶HZSM-5催化性能的影响。通过SEM、XRD、XRF、液体静态吸附、N₂吸附-脱附、NH₃-TPD、Py-FTIR等表征实验对核壳材料的结构和酸性质进行了详细研究。
- 孪晶HZSM-5 /
- Silicalite-1 /
- 核壳结构 /
- 择形催化 /
- 对二甲苯
Abstract: The technology of alkylation of toluene with methanol to p-xylene has attracted much attention due to the high selectivity of p-xylene and low energy consumption in product separation unit. Twin HZSM-5 molecular sieve has the characteristics of large coverage proportion of zigzag channels on the surface and less aluminum distribution on the outer surface. It shows high selectivity for p-xylene in the alkylation of toluene and methanol. In this paper, silicalite-1 (S-1) was grown epitaxially on the surface of twin HZSM-5 molecular sieve by hydrothermal crystallization, and twin HZSM-5@Silicalite-1 core-shell catalyst was obtained. Compared with twin HZSM-5, HZSM-5@40Silicalite-1 core-shell catalyst shows excellent catalytic performance in toluene methanol alkylation. Under the reaction conditions of 470 ℃, 0.1 MPa and hydrogen atmosphere, the conversion of toluene is 8.5% and the selectivity of p-xylene is 98.4%. Then, the effect of solid-liquid mass ratio of nuclear HZSM-5 and silicalite-1 shell precursors on the growth of silicalite-1 crystal was further studied, and the effect of silicalite-1 on the catalytic performance of twin HZSM-5 was investigated. The pore structure and acid properties of core-shell materials were studied in detail by SEM, XRD, XRF, liquid static adsorption, N₂ adsorption desorption, NH₃-TPD and Py-FTIR.
- twin HZSM-5 /
- silicalite-1 /
- core-shell structure /
- shape-selective catalysis /
- para-xylene

HTML全文

FIG. 1529. FIG. 1529.

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图 1 样品的SEM照片：(a) HZSM-5; (b) HZSM-5@10S-1; (c) HZSM-5@20S-1; (d) HZSM-5@40S-1

Figure 1 SEM of the samples: (a) HZSM-5; (b) HZSM-5@10S-1; (c) HZSM-5@20S-1; (d) HZSM-5@40S-1

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图 2 样品的XRD谱图

Figure 2 XRD patterns of the samples

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图 3 样品的液体吸附

Figure 3 Samples liquid adsorption diagram

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图 4 HZSM-5和HZSM-5@S-1的吸附等温线(a)和孔径分布图(b)

Figure 4 Adsorption isotherm (a) and pore size distribution (b) of HZSM-5 and HZSM-5@S-1

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图 5 HZSM-5和HZSM-5@S-1的NH₃-TPD谱图

Figure 5 NH₃-TPD spectra of HZSM-5 and HZSM-5@S-1

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图 6 HZSM-5和HZSM-5@S-1分子筛在350 ℃的Py-FTIR谱图

Figure 6 Py-FTIR spectra of HZSM-5 and HZSM-5@S-1 molecular sieve at 350 ℃

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图 7 样品的甲苯甲醇烷基化催化性能

Figure 7 Catalytic performance of the sample for toluene methanol alkylationa: traditional HZSM-5; b: twin HZSM-5; c: HZSM-5@10S-1;d: HZSM-5@20S-1; e: HZSM-5@40S -1

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表 1 样品的Si/Al物质的量比

Table 1 Molar ratio Si / Al of the samples

Sample	Si/Al（mol ratio）
HZSM-5	152
HZSM-5@10S-1	171
HZSM-5@20S-1	186
HZSM-5@40S-1	199

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表 2 HZSM-5和HZSM-5@S-1分子筛的结构参数

Table 2 Structural properties of HZSM-5 and HZSM-5@S-1 molecular sieves

Sample	${S} _{ {\rm{BET} } }^{\rm{a} } /$(m²·g⁻¹)	${S} _{ {\rm{micro} } }^{\rm{b} } /$(m²·g⁻¹)	${S} _{ {\rm{exter} } }^{\rm{b} } /$(m²·g⁻¹)	${v}_ {\rm{total} } /$(cm³·g⁻¹)	$v_{ {\rm{micro} } }^{\rm{b} } /$(cm³·g⁻¹)	$v_{ {\rm{meso} } }^{\rm{b} }/$(cm³·g⁻¹)
HZSM-5	370	288	82	0.18	0.12	0.06
HZSM-5@10S-1	351	250	101	0.18	0.11	0.07
HZSM-5@20S-1	339	240	99	0.18	0.10	0.08
HZSM-5@40S-1	351	260	91	0.20	0.11	0.09
^a Calculated by the BET method; ^b Calculated using the t-plot method; ^c Calculated using v_total −v_micro

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表 3 探针分子PX、MX和OX的异构转化率

Table 3 isomerization conversion of probe molecules PX, MX and OX

Sample	PX isomerization conversion /%	MX isomerization conversion /%	OX isomerization conversion /%
Black	−	−	−
HZSM-5	3.9	1.6	1.5
HZSM-5@10S-1	1.9	0.7	0.9
HZSM-5@20S-1	1.3	0.4	0.6
HZSM-5@40S-1	0.8	0.1	0.5

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