中国科学院大连化学物理研究所机构知识库
Advanced  
DICP OpenIR  > 中国科学院大连化学物理研究所  > 期刊论文
题名: Hydrogenation of methyl acetate to ethanol over a highly stable Cu/SiO2 catalyst: Reaction mechanism and structural evolution
作者: Huang, Xiumin1;  Ma, Meng1;  Miao, Shu1;  Zheng, Yanping2;  Chen, Mingshu2;  Shen, Wenjie1
关键词: Cu/SiO2 catalyst ;  Core-shell structure ;  Methyl acetate ;  Hydrogenation ;  Stability
刊名: APPLIED CATALYSIS A-GENERAL
发表日期: 2017-02-05
DOI: 10.1016/j.apcata.2016.12.006
卷: 531, 页:79-88
收录类别: SCI
文章类型: Article
WOS标题词: Science & Technology ;  Physical Sciences ;  Life Sciences & Biomedicine
类目[WOS]: Chemistry, Physical ;  Environmental Sciences
研究领域[WOS]: Chemistry ;  Environmental Sciences & Ecology
英文摘要: A Cu/SiO2 catalyst with a core-shell structure was found to be highly active and stable for the hydrogenation of methyl acetate to ethanol during 96 h reaction test at 523 K; MA conversion reached at 95% while the selectivity towards the major products (ethanol and methanol) approached similar to 95%. Structural analysis revealed that most copper particles in the hydrogen-reduced Cu/SiO2 catalyst had sizes of 3-7 nm and were coated with a thin layer of silica, forming a core-shell structure. The average size of copper particles and the core-shell structure kept unchanged in the spent catalyst, but the Cu+/(Cu-0 + Cu+) ratio increased during the course of reaction, probably because of the electronic interaction between copper surface and methyl acetate under the reaction conditions. Mechanistic and kinetic studies have identified that ethyl acetate was formed through trans-esterification of initially produced ethanol with methyl acetate, while the subsequent hydrogenation of ethyl acetate to ethanol proceeded much faster. The Cu+/(Cu-0 + Cu+) ratio played a crucial role in reaction network; MA could adsorb equally on Cu-0 and Cu+ sites while the activation of molecular hydrogen occurs only on the Cu-0 site. Therefore, a rather stable performance could be attained with the increase in the Cu+/(Cu-0 + Cu+) ratio during the course of reaction as long as the reaction is kinetically controlled by MA adsorption. The outstanding stability of the Cu/SiO2 catalyst was ascribed to a combination of geometric and electronic effect. (C) 2016 Elsevier B.V. All rights reserved.
关键词[WOS]: DIMETHYL ETHER CARBONYLATION ;  PRECIPITATION-GEL METHOD ;  SILICA-SUPPORTED COPPER ;  GLYCEROL HYDROGENOLYSIS ;  ETHYLENE-GLYCOL ;  H-MORDENITE ;  CHEMOSELECTIVE HYDROGENATION ;  ACIDIC ZEOLITES ;  OXALATE ;  PERFORMANCE
语种: 英语
WOS记录号: WOS:000392680500010
Citation statistics: 
内容类型: 期刊论文
URI标识: http://cas-ir.dicp.ac.cn/handle/321008/151883
Appears in Collections:中国科学院大连化学物理研究所_期刊论文

Files in This Item:

There are no files associated with this item.


作者单位: 1.Chinese Acad Sci, Dalian Inst Chem Phys, State Key Lab Catalysis, Dalian 116023, Peoples R China
2.Xiamen Univ, Dept Chem, State Key Lab Phys Chem Solid Surfaces, Xiamen 361005, Peoples R China

Recommended Citation:
Huang, Xiumin,Ma, Meng,Miao, Shu,et al. Hydrogenation of methyl acetate to ethanol over a highly stable Cu/SiO2 catalyst: Reaction mechanism and structural evolution[J]. APPLIED CATALYSIS A-GENERAL,2017,531:79-88.
Service
 Recommend this item
 Sava as my favorate item
 Show this item's statistics
 Export Endnote File
Google Scholar
 Similar articles in Google Scholar
 [Huang, Xiumin]'s Articles
 [Ma, Meng]'s Articles
 [Miao, Shu]'s Articles
CSDL cross search
 Similar articles in CSDL Cross Search
 [Huang, Xiumin]‘s Articles
 [Ma, Meng]‘s Articles
 [Miao, Shu]‘s Articles
Related Copyright Policies
Null
Social Bookmarking
  Add to CiteULike  Add to Connotea  Add to Del.icio.us  Add to Digg  Add to Reddit 
所有评论 (0)
暂无评论
 
评注功能仅针对注册用户开放,请您登录
您对该条目有什么异议,请填写以下表单,管理员会尽快联系您。
内 容:
Email:  *
单位:
验证码:   刷新
您在IR的使用过程中有什么好的想法或者建议可以反馈给我们。
标 题:
 *
内 容:
Email:  *
验证码:   刷新

Items in IR are protected by copyright, with all rights reserved, unless otherwise indicated.

 

 

Valid XHTML 1.0!
Powered by CSpace