Direct Conversion of Syngas to Higher Alcohols over a CuCoAl|t-ZrO2 Multifunctional Catalyst

被引:13
|
作者
Huang, Chao [1 ,2 ]
Zhu, Can [1 ,2 ]
Zhang, Mingwei [1 ]
Lu, Yongwu [3 ]
Wang, Qianhao [1 ,2 ]
Qian, Heming [4 ]
Chen, Jiangang [1 ]
Fang, Kegong [1 ]
机构
[1] Chinese Acad Sci, Inst Coal Chem, State Key Lab Coal Convers, Taiyuan 030001, Shanxi, Peoples R China
[2] Univ Chinese Acad Sci, Beijing 100049, Peoples R China
[3] Chinese Acad Sci, Shanghai Adv Res Inst, CAS Key Lab Low Carbon Convers Sci & Engn, Shanghai 201203, Peoples R China
[4] Northeast Petr Univ, Coll Chem & Chem Engn, Daqing 163318, Peoples R China
基金
上海市自然科学基金; 国家重点研发计划; 中国国家自然科学基金;
关键词
CuCoAl|t-ZrO2 Catalyst; Higher Alcohols Synthesis; Synergetic Effect; Structure-Performance Relationship; Reaction Mechanism; FISCHER-TROPSCH SYNTHESIS; ALKALINE-EARTH METALS; CU-CO; SELECTIVE CONVERSION; ISOBUTANOL SYNTHESIS; COBALT CATALYSTS; NI/ZRO2; CATALYST; ZIRCONIA; HYDROGENATION; ETHANOL;
D O I
10.1002/cctc.202100293
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Selective synthesis of higher alcohols from syngas is promising but remains challenging owing to the low stability and selectivity towards higher alcohols. Here we introduce a CuCoAl|t-ZrO2 (t denotes tetragonal crystal phase) multifunctional catalyst that can achieve an alcohol selectivity of 64.8 % with 79.6 % C2+OH, and a total selectivity of alcohols and olefins to 81.7 %. The proper proximity was tuned to increase selectivity towards alcohols and decrease the selectivity towards hydrocarbons. The lower surface [H*]/[C*] ratio due to the stronger basic sites of the CuCoAl|t-ZrO2 limited alkyl (CHx) species hydrogenation, and promoted CO insertion and carbon chain growth, resulting in improving the alcohols selectivity. Meanwhile, the weaker adsorption of bridge-type adsorbed CO and the lower decomposition rate of multi-bonded adsorbed CO over CuCoAl|t-ZrO2 inhibited hydrocarbon generation. The selective promotion of the reaction route via the synergetic effect between CuCoAl and t-ZrO2 was proposed to boost higher alcohols selectivity. This work may aid the rational design of effective multifunctional catalyst with synergistic effects for tuning selectivity.
引用
收藏
页码:3184 / 3197
页数:14
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