蜂窝陶瓷骨架微结构修饰调控制备Pd/CNTs@CHC催化剂用于PS加氢

doi:10.11949/j.issn.0438-1157.20170056

化工学报 ›› 2017, Vol. 68 ›› Issue (7): 2746-2754.DOI: 10.11949/j.issn.0438-1157.20170056

• 催化、动力学与反应器 • 上一篇下一篇

蜂窝陶瓷骨架微结构修饰调控制备Pd/CNTs@CHC催化剂用于PS加氢

李晨阳, 冯淼, 崔海峰, 曹贵平, 吕慧, 陈荣起

华东理工大学联合化学反应工程研究所, 化学工程联合国家重点实验室, 上海 200237

收稿日期:2017-01-13 修回日期:2017-04-26 出版日期:2017-07-05 发布日期:2017-07-05
通讯作者: 曹贵平
基金资助:
国家自然科学基金项目（21576091）；教育部博士学科点专项科研基金项目（20110074110012）；上海市科委国际合作项目（10520706000）；化学工程联合国家重点实验室专项基金项目（SKL-ChE-09C07）；大学生创新项目（x17005，x17009）。

Preparation of carbon nanotube catalyst on structure-modified cordierite monolith for polystyrene hydrogenation

LI Chenyang, FENG Miao, CUI Haifeng, CAO Guiping, LÜ Hui, CHEN Rongqi

State Key Laboratory of Chemical Engineering, UNILAB Research Center of Chemical Reaction Engineering, East China University of Science and Technology, Shanghai 200237, China

Received:2017-01-13 Revised:2017-04-26 Online:2017-07-05 Published:2017-07-05
Contact: 10.11949/j.issn.0438-1157.20170056
Supported by:
supported by the National Natural Science Foundation of China (21576091), the PhD Program Foundation of Ministry and Education of China (20110074110012), the Non-governmental International Science and Technology Cooperation Program from the Science and Technology Commission of Shanghai Municipality (10520706000), the State Key Laboratory of Chemical Engineering Open Fund (SKL-ChE-09C07) and the College Students Innovative Entrepreneurial Training Plan Program of East China University of Science and Technology (x17005, x17009).

摘要/Abstract

摘要：

通过高温焙烧和氢氟酸瞬间蚀刻修饰堇青石蜂窝陶瓷骨架和孔壁表面结构，采用XRD、SEM、TEM表征修饰前后结构和形貌变化，探究陶瓷结构对机械强度、碳纳米管形貌结构及复合载体性质的影响，考察Pd/CNTs@CHC-HFn催化剂催化聚苯乙烯（PS）加氢性能及催化剂用量与加氢度的关系。结果表明，高温焙烧消除了骨架内部孔道，陶瓷表面变得平整密实；瞬间蚀刻增大了表面粗糙度，易于CNTs在表面生长，但蚀刻次数增加，导致蚀刻由表面向骨架内部侵入、CNTs在骨架内部生长，降低载体的机械强度。CNTs@CHC-HFn载体表面的CNTs可显著提高复合催化剂的加氢性能，其中加氢活性位Pd分布均匀，平均粒径为3.6 nm，当催化剂用量为3.0 g cat·（g PS）^-1时，其中含0.378 g CNTs和0.054 g Pd，反应6 h加氢度可达100%。

关键词: 堇青石陶瓷, 整体式催化剂, 碳纳米管, 聚苯乙烯, 催化加氢

Abstract:

Cordierite honeycomb ceramic (CHC) was modified by high-temperature calcination and hydrofluoric acid instantaneous etching. The framework microstructures and pore surface morphologies before and after treatment were characterized using SEM, XRD and TEM. The effect of ceramic structure on mechanical strength, morphology of carbon nanotubes, and property of complex carrier were studied. Catalytic performance of Pd/CNTs@CHC-HFn and amount of catalyst on degree of polystyrene hydrogenation were evaluated. High-temperature calcination eliminated internal pores of ceramic framework and ceramic surface became flat and dense. Instantaneous etching increased surface roughness and facilitated CNT growth on the surface. However, increase of etching cycles reduced mechanical strength of carriers as a result of over-etching into framework and CNT growth inside framework pores. CNTs growing on modified CHC-HFn surface significantly improved homogeneous dispersion of palladium and subsequently enhanced hydrogenation performance. The average particle size of palladium was 3.6 nm in the complex catalyst. At catalyst amount of 3.0 g cat·(g PS)^-¹, which contained 0.378 g CNTs and 0.054 g Pd, the degree of hydrogenation for polystyrene to poly(vinylcyclohexane) reached up to 100% in 6 h reaction time.

Key words: cordierite monolith, monolithic catalyst, carbon nanotubes, polystyrene, catalytic hydrogenation

中图分类号:

TQ426.94

李晨阳, 冯淼, 崔海峰, 曹贵平, 吕慧, 陈荣起. 蜂窝陶瓷骨架微结构修饰调控制备Pd/CNTs@CHC催化剂用于PS加氢[J]. 化工学报, 2017, 68(7): 2746-2754.

LI Chenyang, FENG Miao, CUI Haifeng, CAO Guiping, LÜ Hui, CHEN Rongqi. Preparation of carbon nanotube catalyst on structure-modified cordierite monolith for polystyrene hydrogenation[J]. CIESC Journal, 2017, 68(7): 2746-2754.

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蜂窝陶瓷骨架微结构修饰调控制备Pd/CNTs@CHC催化剂用于PS加氢

Preparation of carbon nanotube catalyst on structure-modified cordierite monolith for polystyrene hydrogenation

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