水滑石基钴铜催化剂中钴的碳化在高碳醇合成中的作用

doi:10.1016/S1872-2067(19)63344-9

催化学报 ›› 2019, Vol. 40 ›› Issue (11): 1731-1740.DOI: 10.1016/S1872-2067(19)63344-9

水滑石基钴铜催化剂中钴的碳化在高碳醇合成中的作用

Janine Nebel^a, Stefan Schmidt^a, Qiushi Pan^a, Katrin Lotz^a, Stefan Kaluza^a,b, Martin Muhler^a

a 波鸿鲁尔大学工业化学实验室, 波鸿 44780, 德国;
b 弗劳恩霍夫环境安全与能源技术研究所, 奥伯豪森 46047, 德国

收稿日期:2019-01-25 修回日期:2019-03-07 出版日期:2019-11-18 发布日期:2019-09-06
通讯作者: Stefan Kaluza, Martin Muhler
基金资助:
The research project is funded by the Federal Ministry of Education and Research (Bundesministerium für Bildung und Forschung, BMBF, Ver-bundvorhaben Carbon2Chem^®, FKZ:03EK3041).

On the role of cobalt carbidization in higher alcohol synthesis over hydrotalcite-based Co-Cu catalysts

Janine Nebel^a, Stefan Schmidt^a, Qiushi Pan^a, Katrin Lotz^a, Stefan Kaluza^a,b, Martin Muhler^a

a Laboratory of Industrial Chemistry, Ruhr-University Bochum, Universitätsstr. 150, 44780 Bochum, Germany;
b Fraunhofer Institute for Environmental, Safety, and Energy Technology UMSICHT, Osterfelder Str. 3, 46047 Oberhausen, Germany

Received:2019-01-25 Revised:2019-03-07 Online:2019-11-18 Published:2019-09-06
Contact: Stefan Kaluza, Martin Muhler
Supported by:
The research project is funded by the Federal Ministry of Education and Research (Bundesministerium für Bildung und Forschung, BMBF, Ver-bundvorhaben Carbon2Chem®, FKZ:03EK3041).

摘要/Abstract

摘要： Co-Cu基催化剂广泛用于合成气制高碳醇反应（HAS）中.尽管很难从本质上完全理解催化剂的活性位，但是在HAS条件下生成的Co₂C对反应的贡献是显而易见的.开发了CO预处理工艺，系统地研究了钴的碳化对催化剂结构性能和催化性能的影响.通过在HAS反应之前将催化剂暴露在含CO的气氛中，催化剂表面发生Co的富集，然后形成碳化物.这种表面改性减少了烃类的形成，促进了C₂₊OH的形成.催化剂经20 bar下CO预处理后，乙醇选择性最高，烃类选择性最低.

关键词: 高碳醇合成, Co-Cu催化剂, 碳化钴, CO预处理

Abstract: Co-Cu-based catalysts are widely applied in higher alcohol synthesis (HAS) from synthesis gas. Although the nature of the active sites is still not fully understood, the formation of Co₂C under HAS conditions seems to play a major role. A CO pretreatment procedure was developed allowing a systematic investigation of the influence of cobalt carbidization on the structural properties and catalytic performance of the catalysts. By exposing the catalyst to a CO-containing atmosphere prior to HAS, Co enrichment of the catalyst surface occurred followed by carbide formation. This surface modification decreased the formation of hydrocarbons and enhanced the formation of C₂₊OH. The catalyst pretreated with CO at 20 bar achieved the highest selectivity to ethanol and the lowest hydrocarbon selectivity.

Key words: Higher alcohol synthesis, Co-Cu catalyst, Co₂C, CO pretreatment

Janine Nebel, Stefan Schmidt, Qiushi Pan, Katrin Lotz, Stefan Kaluza, Martin Muhler. 水滑石基钴铜催化剂中钴的碳化在高碳醇合成中的作用[J]. 催化学报, 2019, 40(11): 1731-1740.

Janine Nebel, Stefan Schmidt, Qiushi Pan, Katrin Lotz, Stefan Kaluza, Martin Muhler. On the role of cobalt carbidization in higher alcohol synthesis over hydrotalcite-based Co-Cu catalysts[J]. Chinese Journal of Catalysis, 2019, 40(11): 1731-1740.

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水滑石基钴铜催化剂中钴的碳化在高碳醇合成中的作用

On the role of cobalt carbidization in higher alcohol synthesis over hydrotalcite-based Co-Cu catalysts

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