Au/SiO2-Based Catalysts for Propanol/Propanal Synthesis from CO2, C2H4, and H2 in a Dual-reactor System

被引:3
作者
Truong, Duc Duc [1 ]
Pham, Phuong Thi Mai [2 ]
V. Kondratenko, Evgenii [3 ]
Le, Minh Thang [1 ]
机构
[1] Hanoi Univ Sci & Technol, Sch Chem Engn, Hanoi 100000, Vietnam
[2] Hanoi Univ Sci & Technol, Int Training Inst Mat Sci, Hanoi 100000, Vietnam
[3] Leibniz Inst Katalyse eV LIKAT, D-18059 Rostock, Germany
关键词
hydroformylation; gold; SiO2; propanol; propanal; dual reactor; ETHYLENE HYDROFORMYLATION; PROPANOL SYNTHESIS; HYDROGENATION; TEMPERATURE; PROMOTER; WATER; RH;
D O I
10.1021/acssuschemeng.2c03992
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
CO2 hydrogenation to value-added products is a promising approach for controlling CO2 emissions into the atmosphere. In this work, we introduce and validate a dual-reactor approach for improving the oxo-selectivity (propanol plus propanal) in the direct production of these oxygenates from C2H4, CO2, and H2 over SiO2-supported Au-containing catalysts. The reverse water gas shift reaction was performed at high temperatures in the upstream-located reactor, while the hydroformylation reaction of ethylene was carried out at lower temperatures in the downstream-located reactor without the need for expensive preseparation of the product mixture from the first reactor. Both reactors operated at the same pressure. The effects of temperature, total pressure, and the ratio of CO/H2 adjusted through temperature in the upstream-located reactor, as well as the Au loading content and the Cs doping content on the catalytic activity and oxo-selectivity were investigated. The highest oxo-selectivity of 60% at ethylene conversion of 15% was achieved. The size of Au crystallites was established to be an important selectivity-governing factor. This catalyst characteristic depends on Au loading and Cs presence.
引用
收藏
页码:16548 / 16554
页数:7
相关论文
共 23 条
[1]   Direct propanol synthesis from CO2, C2H4, and H2 over Cs-Au/TiO2 rutile: effect of promoter loading, temperature and feed composition [J].
Ahlers, S. J. ;
Pohl, M. -M. ;
Holena, M. ;
Linke, D. ;
Kondratenko, E. V. .
CATALYSIS SCIENCE & TECHNOLOGY, 2016, 6 (07) :2171-2180
[2]  
Ahlers S. J., 2016, THESIS ROSTOCK U
[3]   Propanol formation from CO2 and C2H4 with H2 over Au/TiO2: Effect of support and K doping [J].
Ahlers, Stefan J. ;
Kraehnert, Ralph ;
Kreyenschulte, Carsten ;
Pohl, Marga-Martina ;
Linke, David ;
Kondratenko, Evgenii V. .
CATALYSIS TODAY, 2015, 258 :684-690
[4]   Catalytic role and location of Cs promoter in Cs-Au/TiO2 catalysts for propanol synthesis from CO2, C2H4 and H2 [J].
Ahlers, Stefan J. ;
Pohl, Marga-Martina ;
Radnik, Joerg ;
Linke, David ;
Kondratenko, Evgenii V. .
APPLIED CATALYSIS B-ENVIRONMENTAL, 2015, 176 :570-577
[5]   An Innovative Approach for Highly Selective Direct Conversion of CO2 into Propanol using C2H4 and H2 [J].
Ahlers, Stefan J. ;
Bentrup, Ursula ;
Linke, David ;
Kondratenko, Evgenii V. .
CHEMSUSCHEM, 2014, 7 (09) :2631-2639
[6]  
Alsalahi W, 2021, COORDIN CHEM REV, V430, P13732
[7]   Towards Solar Fuels from Water and CO2 [J].
Centi, Gabriele ;
Perathoner, Siglinda .
CHEMSUSCHEM, 2010, 3 (02) :195-208
[8]   Transformation of Carbon Dioxide with Homogeneous Transition-Metal Catalysts: A Molecular Solution to a Global Challenge? [J].
Cokoja, Mirza ;
Bruckmeier, Christian ;
Rieger, Bernhard ;
Herrmann, Wolfgang A. ;
Kuehn, Fritz E. .
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2011, 50 (37) :8510-8537
[9]   State-of-the-Art Catalysts for Hydrogenation of Carbon Dioxide [J].
Federsel, Christopher ;
Jackstell, Ralf ;
Beller, Matthias .
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2010, 49 (36) :6254-6257
[10]   Ethylene hydroformylation and carbon monoxide hydrogenation over modified and unmodified silica supported rhodium catalysts [J].
Hanaoka, T ;
Arakawa, H ;
Matsuzaki, T ;
Sugi, Y ;
Kanno, K ;
Abe, Y .
CATALYSIS TODAY, 2000, 58 (04) :271-280