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

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 ...

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Veröffentlicht in:ChemCatChem 2021-07, Vol.13 (13), p.3184-3197
Hauptverfasser: Huang, Chao, Zhu, Can, Zhang, Mingwei, Lu, Yongwu, Wang, Qianhao, Qian, Heming, Chen, Jiangang, Fang, Kegong
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container_issue 13
container_start_page 3184
container_title ChemCatChem
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creator Huang, Chao
Zhu, Can
Zhang, Mingwei
Lu, Yongwu
Wang, Qianhao
Qian, Heming
Chen, Jiangang
Fang, Kegong
description 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. Synergetic effect: The physically mixed CuCoAl|t‐ZrO2 multifunctional catalyst could achieve superior selectivity towards alcohols while simultaneously inhibiting the generation of hydrocarbons from CO hydrogenation.
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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. 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source Wiley Online Library Journals Frontfile Complete
subjects Alcohol
Alcohols
Alkenes
Carbon monoxide
Catalysts
CuCoAl|t-ZrO2 Catalyst
Direct conversion
Higher Alcohols Synthesis
Hydrocarbons
Molecular chains
Reaction Mechanism
Selectivity
Structure-Performance Relationship
Synergetic Effect
Synergistic effect
Synthesis gas
Zirconium dioxide
title Direct Conversion of Syngas to Higher Alcohols over a CuCoAl|t‐ZrO2 Multifunctional Catalyst
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