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[1]陈秋虹,张梦辉,林国栋,等.由(CO2+H2)直接合成二甲醚用的CNT促进Cu-ZrO2-HZSM-5混合型催化剂[J].厦门大学学报(自然科学版),2012,51(6):1036.
 CHEN Qiu-hong,ZHANG Meng-hui,LIN Guo-dong,et al.CNT-promoted Cu-ZrO2-HZSM-5 Hybrid Catalysts for Direct Synthesis of DME from(CO2+H2)[J].Journal of Xiamen University(Natural Science),2012,51(6):1036.
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《厦门大学学报(自然科学版)》[ISSN:0438-0479/CN:35-1070/N]

卷:
51卷
期数:
2012年第6期
页码:
1036
栏目:
研究论文
出版日期:
2012-11-30

文章信息/Info

Title:
CNT-promoted Cu-ZrO2-HZSM-5 Hybrid Catalysts for Direct Synthesis of DME from(CO2+H2)
作者:
陈秋虹张梦辉林国栋张鸿斌*
厦门大学 化学化工学院,固体表面物理化学国家重点实验室,醇醚酯化工清洁生产国家工程实验室,福建 厦门 361005
Author(s):
CHEN Qiu-hong ZHANG Meng-hui LIN Guo-dong ZHANG Hong-bin*
State Key Laboratory of Physical Chemistry of Solid Surfaces,National Engineering Laboratory for Green Chemical Productions of Alcohols-Ethers-Esters,College of Chemistry and Chemical Engineering,Xiamen University,Xiamen 361005,China
关键词:
多壁碳纳米管 CNT促进Cu-ZrO2-HZSM-5双功能混合型催化剂 CO2加氢 二甲醚合成
Keywords:
MWCNTs CNT-promoted Cu-ZrO2-HZSM-5 bi-functional hybrid catalyst CO2 hydrogenation DME synthesis
分类号:
O 643.36
文献标志码:
A
摘要:
CO2加氢被认为是目前固定大量排放CO2的最好方法之一.研发出一种碳纳米管(CNT)促进的Cu-ZrO2-HZSM-5沸石分子筛双功能混合型催化剂, 将其用于CO2加氢合成甲醇和甲醇脱水生成二甲醚(DME)二步串联催化一器化,实现由(CO2+H2)直接合成DME.在5.0 MPa,523 K,V(H2):V(CO2):V(N2)= 69:23:8,空速(GHSV)=25 000 mL/(h·g)的反应条件下,在所研发(Cu2Zr3-10%CNT)-30%HZSM-5催化剂上,CO2加氢的转化率达9.44%,比相应单功能加氢催化剂(Cu2Zr3-10%CNT)的相应值(7.00%)提高35%.CNT能作为Cu-ZrO2-HZSM-5双功能混合型催化剂的促进剂.在上述反应条件下,含CNT的催化剂的DME时空产率达438 mg/(h·g),比不含CNT的原双功能混合型基质催化剂的相应值(395 mg/(h·g))提高11%.结果证实,利用双功能混合型催化剂,将CO2加氢合成甲醇和甲醇脱水生成DME两个过程串联催化一器化,能大幅度提高CO2加氢转化的效率.
Abstract:
In order to improve the climate conditions,it is desirable to develop methods to convert CO2 into valuable chemicals.Here we report the development of a CNT-promoted Cu-ZrO2-HZSM-5 bi-functional hybrid catalyst,which was used for the “one-pot” two-step catalytic synthesis of DME from(CO2+H2)via CH3OH.Over the developed catalyst of(Cu2Zr3-10%CNT)-30%HZSM-5 under the reaction conditions of 5.0 MPa,523 K,V(H2):V(CO2):V(N2)=69:23:8,GHSV=25 000 mL/(h·g),the CO2 hydrogenation conversion reached 9.44%.This value was 1.35 times that(7.00%)of the mono-functional hydrogenation catalyst of Cu2Zr3-10%CNT.The CNT could act as a novel promoter of the Cu-ZrO2-HZSM-5 bi-functional hybrid catalyst.Under the aforementioned reaction conditions,the space-time-yield(STY)of DME reached 438 mg/(h·g)over the CNT-containing bi-functional hybrid catalyst,which was 1.11 times that(395 mg/(h·g))of the corresponding CNT-free counterpart.The results of the present work demonstrated that combination of the process for methanol synthesis with that for methanol dehydration to produce DME by using bi-functional hybrid catalyst could markedly improve the efficiency of CO2 hydrogenation-conversion.

参考文献/References:


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备注/Memo

备注/Memo:
收稿日期:2012-05-24
基金项目:国家重点基础研究发展计划(973)项目(2011CBA00508); 优秀国家重点实验室研究项目基金(20923004); 教育部创新团队项目(IRT1036)和福建省重大专项专题项目(2009HZ0002-1)
更新日期/Last Update: 2012-11-20