碱改性HZSM-5催化热解木质素催化剂失活分析

doi:10.11949/j.issn.0438-1157.20170764

化工学报 ›› 2017, Vol. 68 ›› Issue (12): 4739-4749.DOI: 10.11949/j.issn.0438-1157.20170764

碱改性HZSM-5催化热解木质素催化剂失活分析

唐松山^1,3, 泮泽优^1,2, 张长森^1,2, 王登台^1,2, 薛翔飞^1,2, 曹云峰³, 刘永刚^1,2, 张瑞芹^1,2

1 郑州大学化学与分子工程学院, 河南郑州 450001;
2 河南省环境化学与低碳技术重点实验室, 河南郑州 450001;
3 天方药业有限公司, 河南驻马店 463000

收稿日期:2017-06-13 修回日期:2017-07-18 出版日期:2017-12-05 发布日期:2017-12-05
通讯作者: 张长森
基金资助:
河南省国际合作基金项目（172102410041）。

Deactivation analysis of catalyst for modified HZSM-5 catalytic lignin pyrolysis

TANG Songshan^1,3, PAN Zeyou^1,2, ZHANG Changsen^1,2, WANG Dengtai^1,2, XUE Xiangfei^1,2, CAO Yunfeng³, LIU Yonggang^1,2, ZHANG Ruiqin^1,2

1 College of Chemistry and Molecular Engineering, Zhengzhou University, Zhengzhou 450001, Henan, China;
2 Environmental Chemistry & Low Carbon Technologies Key Laboratory of Henan Province, Zhengzhou 450001, Henan, China;
3 Topfond Pharmaceutical Co., Ltd., Zhumadian 463000, Henan, China

Received:2017-06-13 Revised:2017-07-18 Online:2017-12-05 Published:2017-12-05
Supported by:
supported by the International Cooperation Science Foundation of Henan Province (172102410041).

摘要/Abstract

摘要：

对0.3 mol·L^-1 NaOH改性后的HZSM-5以及未改性HZSM-5催化剂进行循环和再生评价实验以考察催化剂的寿命。对反应后和再生的催化剂进行N₂吸脱附以及NH₃-TPD表征，并通过对反应后的催化剂进行SEM、TGA、FTIR、UV-Vis等表征分析催化剂积炭。两种催化剂的活性均随着循环实验次数的增加而逐渐降低，经4次循环实验的改性HZSM-5催化剂的催化活性远高于4次循环实验的未改性HZSM-5催化剂。反应过的催化剂经高温煅烧再生后其活性都有所恢复，再生后的改性HZSM-5的催化活性仍高于未改性催化剂。对两种不同催化剂积炭分析，改性后催化剂的积炭量少于未改性的催化剂，其积炭组分中高聚芳烃的含量相对较多。

关键词: HZSM-5分子筛, 催化热解, 木质素, 失活, 再生, 积炭

Abstract:

The circulation and regeneration experiments were employed to evaluate the lifetime of the two different catalysts (HZSM-5 and 0.3 mol·L^-1 NaOH modified HZSM-5). The spent and regenerated catalysts were characterized by N₂ adsorption-desorption and NH₃-TPD techniques to analyse the reason of deactivation, and the spent catalysts were characterized by SEM,TGA, FTIR and UV-Vis techniques to analyse the coke deposited on the catalyst. The deactivation of the two different zeolites was become more and more serious along with the increase of the number of cycles. The difference was that the performance of 0.3 mol·L^-1 NaOH modified HZSM-5 was better than the one of unmodified HZSM-5 after four cycles. The coke of the spent catalysts was removed through calcination in air at high temperature and the catalytic activity was recovered to a large extent. The performance of 0.3 mol·L^-1 NaOH modified HZSM-5 was still better than the one of unmodified HZSM-5 after regeneration. The amount of coke deposited on the modified HZSM-5 was less than the one of unmodified HZSM-5. The coke of the modified HZSM-5 contains more condensed aromatics relatively.

Key words: HZSM-5 zeolites, catalytic pyrolysis, lignin, deactivation, regeneration, coke

中图分类号:

TQ032.4

唐松山, 泮泽优, 张长森, 王登台, 薛翔飞, 曹云峰, 刘永刚, 张瑞芹. 碱改性HZSM-5催化热解木质素催化剂失活分析[J]. 化工学报, 2017, 68(12): 4739-4749.

TANG Songshan, PAN Zeyou, ZHANG Changsen, WANG Dengtai, XUE Xiangfei, CAO Yunfeng, LIU Yonggang, ZHANG Ruiqin. Deactivation analysis of catalyst for modified HZSM-5 catalytic lignin pyrolysis[J]. CIESC Journal, 2017, 68(12): 4739-4749.

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碱改性HZSM-5催化热解木质素催化剂失活分析

Deactivation analysis of catalyst for modified HZSM-5 catalytic lignin pyrolysis

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