成型条件对Co/ZSM-5催化剂催化分解N2O性能影响

doi:10.16085/j.issn.1000-6613.2018-0943

化工进展 ›› 2019, Vol. 38 ›› Issue (04): 1746-1752.DOI: 10.16085/j.issn.1000-6613.2018-0943

成型条件对Co/ZSM-5催化剂催化分解N₂O性能影响

李思漩^1,²(),夏蕾¹,李靖宇¹,刘晓刚¹,孙巾茹^1,³,迟姚玲¹,王虹¹(),李翠清¹,宋永吉¹

1. 北京石油化工学院化学工程学院，燃料清洁化及高效催化减排技术北京市重点实验室，北京 102617
2. 北京化工大学化学工程学院，北京 100029
3. 北京工业大学环境与能源工程学院，北京 100124

收稿日期:2018-05-08 修回日期:2018-09-12 出版日期:2019-04-05 发布日期:2019-04-05
通讯作者: 王虹
作者简介:<named-content content-type="corresp-name">李思漩</named-content>（1989—），女，硕士研究生，研究方向为工业催化。E-mail：<email>1302680058@qq.com</email>。|王虹，教授，硕士生导师，研究方向为工业催化。E-mail：<email>wanghong@bipt.edu.cn</email>。
基金资助:
国家自然科学基金(21343009，U1662103，21673290);燃料清洁化及高效催化减排技术北京市重点实验室项目(BZ041420180007);北京市大学生创新创业训练计划(2018J00035)

Effect of forming conditions on the performance of catalytic decomposition of N₂O over Co/ZSM-5 catalyst

Sixuan LI^1,²(),Lei XIA¹,Jingyu LI¹,Xiaogang LIU¹,Jinru SUN^1,³,Yaoling CHI¹,Hong WANG¹(),Cuiqing LI¹,Yongji SONG¹

1. Beijing Key Laboratory of Fuels Cleaning and Advanced Catalytic Emission Reduction Technology, College of Chemical Engineering, Beijing Institute of Petrochemical Technology, Beijing Institute of Petrochemical Technology, Beijing 102617, China
2. College of Chemical Engineering, Beijing University of Chemical Technology, Beijing 100029, China
3. College of Environmental and Energy Engineering, Beijing University of Technology, Beijing 100124, China

Received:2018-05-08 Revised:2018-09-12 Online:2019-04-05 Published:2019-04-05
Contact: Hong WANG

摘要/Abstract

摘要：

采用挤条成型法制备Co/ZSM-5催化剂，通过X射线衍射、BET比表面积、氢气程序升温还原（H₂-TPR）、氨气程序升温脱附法（NH₃-TPD）和颗粒径向抗压碎（侧压）强度测试对催化剂进行表征，在固定床微型反应器中评价催化剂催化分解N₂O活性，对Co/ZSM-5(N-50)催化剂进行稳定性测试。结果表明，钴物种以Co₃O₄尖晶石氧化物形式存在于Co/ZSM-5催化剂中，胶溶剂种类显著影响催化剂抗压碎强度；黏合剂用量影响催化剂抗压碎强度、酸量、氧化还原性和催化剂催化分解N₂O活性；以硝酸为胶溶剂，黏合剂（SB粉）用量为30%和50%制备的催化剂，抗压碎强度大，分别为208N/cm和230N/cm，催化分解N₂O温度T ₉₅分别为485℃和500℃。在固定床微型反应器中，模拟工业尾气组成（ $φ N 2 O$ =11%、 $φ O 2$ =16%、N₂为平衡气），反应温度446℃、空速6000h^-1条件下，Co/ZSM-5(N-50)催化剂在1000h稳定性测试中表现出良好的催化活性和稳定性，N₂O转化率高于98%。

关键词: 催化剂, 钴, 成型条件, 力学性能, N₂O分解

Abstract:

The Co/ZSM-5 catalysts were prepared by extruding strip forming method and were characterized by XRD, BET, H₂-TPR, NH₃-TPD and particle radial crushing (side pressure) strength tests. The activity stability tests of the catalysts for catalytic decomposition of N₂O were carried out in a fixed-bed micro reactor. It was found that the cobalt spices in the catalysts were Co₃O₄and the type of peptizers obviously influenced the mechanical strength of catalysts. The amount of adhesive also influenced the mechanical strength, the amount of acid centers, redox properties and the activities of the catalysts. Co/ZSM-5(N-50) catalyst was prepared with nitric acid as peptizer and SB powder (mass fraction of 30% and 50%) as adhesive. It has strong mechanical strength (208N/cm and 230N/cm, respectively) and the T ₉₅ for N₂O decomposition were 485℃ and 500℃, respectively. Under the simulated industrial tail gas (φ $N 2 O$ =11%, φ $O 2$ =16% and N₂ as balance gas) condition, when the reaction temperature was 446℃ and space velocity was 6000h^-1 in the fixed-bed micro reactor, the Co/ZSM-5(N-50) catalyst showed prominent stability, and the N₂O decomposition conversion was above 98% in a 1000h test.

Key words: catalysts, cobalt, the conditions of molding, mechanical properties, catalytic decomposition of N₂O

中图分类号:

TQ426.68

李思漩, 夏蕾, 李靖宇, 刘晓刚, 孙巾茹, 迟姚玲, 王虹, 李翠清, 宋永吉. 成型条件对Co/ZSM-5催化剂催化分解N₂O性能影响[J]. 化工进展, 2019, 38(04): 1746-1752.

Sixuan LI, Lei XIA, Jingyu LI, Xiaogang LIU, Jinru SUN, Yaoling CHI, Hong WANG, Cuiqing LI, Yongji SONG. Effect of forming conditions on the performance of catalytic decomposition of N₂O over Co/ZSM-5 catalyst[J]. Chemical Industry and Engineering Progress, 2019, 38(04): 1746-1752.

图/表 10

图1 Co/ZSM-5(N-50)三叶草型催化剂图

图2 Co/ZSM-5(P-50)催化剂XRD谱图

图3 胶溶剂对Co/ZSM-5(P-50)催化剂抗压碎强度的影响

图4 胶溶剂对Co/ZSM-5(P-50)催化剂分解N2O活性的影响

图5 黏合剂质量分数对Co/ZSM-5(N-x)催化剂抗压碎强度的影响

图6 Co/ZSM-5(N-x)催化剂H2-TPR谱图

图7 Co/ZSM-5(N-x)催化剂NH3-TPD谱图

图8 黏合剂质量分数对Co/ZSM-5(N-x)催化剂分解N2O活性的影响

图9 Co/ZSM-5(N-50)催化剂分解N2O稳定性试验

表1 稳定性试验前后Co/ZSM-5(N-50)催化剂BET结果

催化剂

比表面积

/m²?g^-1

总孔容

/cm³?g^-1

平均孔径

/nm

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成型条件对Co/ZSM-5催化剂催化分解N₂O性能影响

Effect of forming conditions on the performance of catalytic decomposition of N₂O over Co/ZSM-5 catalyst

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