炭黑颗粒及氟粒子辅助法合成多级结构MCM-22分子筛及其催化性能

doi:10.1016/S1872-2067(12)60711-6

催化学报 ›› 2014, Vol. 35 ›› Issue (1): 49-57.DOI: 10.1016/S1872-2067(12)60711-6

炭黑颗粒及氟粒子辅助法合成多级结构MCM-22分子筛及其催化性能

杨建华, 初筠, 王金渠, 殷德宏, 鲁金明, 张艳

大连理工大学精细化工国家重点实验室, 吸附与无机膜研究所, 辽宁大连 116024

收稿日期:2013-06-28 修回日期:2013-09-04 出版日期:2013-12-23 发布日期:2014-01-17
通讯作者: 杨建华
基金资助:
国家科技支撑计划（2006BAE02B05）；国家自然科学基金（21076029）；新世纪优秀人才支持计划（NCET-10-0286）

Synthesis and catalytic performance of hierarchical MCM-22 zeolite aggregates with the assistance of carbon particles and fluoride ions

Jianhua Yang, Jun Chu, Jinqu Wang, Dehong Yin, Jinming Lu, Yan Zhang

State Key Laboratory of Fine Chemicals, Institute of Adsorption and Inorganic Membranes, School of Chemical Engineering, Dalian University of Technology, Dalian 116024, Liaoning, China

Received:2013-06-28 Revised:2013-09-04 Online:2013-12-23 Published:2014-01-17
Contact: Jianhua Yang
Supported by:
This work was supported by the National Key Technology R&D Program (2006BAE02B05), the National Natural Science Foundation of China (21076029), and the Program for New Century Excellent Talents in University (NCET-10-0286).

摘要/Abstract

摘要：

以碳黑为第二模板剂在氟离子体系中一步水热合成了多级结构MCM-22分子筛组装体（简称为MCM-22-FC）。考察了碳黑和氟离子对MCM-22分子筛形貌和催化性能的影响。MCM-22-FC分子筛是由大量片状晶体交错生长形成的组装体结构，其中MCM-22的片层结构更薄，在其固有的微孔中存在的晶间孔呈现大孔和介孔的特征。MCM-22-FC负载Mo后得到的Mo/MCM-22-FC催化剂在甲烷无氧芳构化反应（MDA）中提高了苯收率和芳烃选择性，并且提高了催化剂的寿命。通过氨气程序升温脱附（NH₃-TPD）表征，吡啶红外（Py-IR）表征，结合热重（TG）分析，得出的结论是Mo/MCM-22-FC在MDA中优越的催化性能是由于氟离子进入到分子筛骨架当中，形成具有拉电子效应的结构单元，从而提高了分子筛的Brönsted酸量，较多的Brönsted酸性位将更多的Mo物种迁移至分子筛孔道内部，形成更多的MoC_x或MoO_xC_y活性物种以及更有利于大分子产物扩散的MCM-22薄片层的结构。少量过剩的Brönsted酸性位在成型后保留在Mo/HMCM-22-FC催化剂活性中心抑制了积碳的形成，也有助于改善芳烃的选择性。

关键词: 甲烷芳构化, MCM-22分子筛, 多级孔道, 氟路线, 催化性能

Abstract:

Hierarchical MCM-22 zeolite aggregates (MCM-22-FC) were prepared by one-pot hydrothermal synthesis with the assistance of carbon particles and fluoride ions. The effects of carbon particles and fluoride ions on the morphology and catalytic properties of the MCM-22 zeolite were investigated. The hierarchical MCM-22-FC zeolite aggregates were constructed by intergrown and stacked thin MCM-22 lamellas and possessed macro-/mesopores and inherent micropores. The MCM-22-FC zeolite was modified to form the Mo/MCM-22-FC catalyst, which exhibited an improved benzene yield and aromatic selectivity as well as catalyst life in the methane dehydroaromatization (MDA) reaction. Based on NH₃-TPD and pyridine-Fourier transform infrared spectroscopy measurements together with thermogravimetric analysis, we found that the improved MDA catalytic performance of Mo/MCM-22-FC resulted from the formation of more active MoC_x or MoO_xC_y species that evolved from increased amounts of Brönsted acids with the assistance of fluoride ions. This promoted the diffusion of large molecule products because of the thin MCM-22 lamellas. Less excess Brönsted acid sites were retained in the Mo/HMCM-22-FC catalyst because the formation of active centers inhibited the formation of coke, which contributed to its improved aromatic selectivity.

Key words: Methane dehydroaromatization, MCM-22 zeolite, Hierarchical pore, Fluoride route, Catalytic performance

杨建华, 初筠, 王金渠, 殷德宏, 鲁金明, 张艳. 炭黑颗粒及氟粒子辅助法合成多级结构MCM-22分子筛及其催化性能[J]. 催化学报, 2014, 35(1): 49-57.

Jianhua Yang, Jun Chu, Jinqu Wang, Dehong Yin, Jinming Lu, Yan Zhang. Synthesis and catalytic performance of hierarchical MCM-22 zeolite aggregates with the assistance of carbon particles and fluoride ions[J]. Chinese Journal of Catalysis, 2014, 35(1): 49-57.

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炭黑颗粒及氟粒子辅助法合成多级结构MCM-22分子筛及其催化性能

Synthesis and catalytic performance of hierarchical MCM-22 zeolite aggregates with the assistance of carbon particles and fluoride ions

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