Abstract
Transition metal modified Rh-catalysts can be used for converting syngas (CO + H2) into C2 + oxygenates. It has been found that Mn has a favorable effect in the selectivity towards oxygenates, while addition of Ir to the binary Rh–Mn catalysts significantly increases the space–time-yield (STY) of C2 + oxygenates, mainly by formyl formation at the early stages of conversion. Quantum mechanical calculations used to investigate the distribution of promoter sites in Rh-rich nanoparticles show that moderately high Mn/Ir ratios result in particles with all 3 metals on the surface, and that Ir atoms act as co-adsorption sinks of CO and H leading to HCO in the initial stages.
This is a preview of subscription content, log in via an institution to check access.
Similar content being viewed by others
References
Ahmed A (2007) Biotechnol Bioeng 97:1080
Spivey JJ, Egbebi A (2007) Chem Soc Rev 36
Burch R, Petch MI (1992) Appl Catal A Gen 88(1):61
Burch R, Petch MI (1992) Appl Catal A Gen 88(1):77
Ichikawa M (1978) Bull Chem Soc Jpn 51(8):2273
Ichikawa M (1978) J Chem Soc Chem Commun 13:566
Underwood RP, Bell AT (1986) Appl Catal 21(1):157
Underwood RP, Bell AT (1987) Appl Catal 34(1–2):289
Gerber MA, Gray MJ, Stevens DJ, White JF, Rummel BL (2010) Optimization of rhodium-based catalysts for mixed alcohol synthesis 2009 progress report. PNNL, Richland, WA
Gerber MA, White JF, Gray MJ, Stevens DJ (2010) Evaluation of promoters for rhodium-based catalysts for mixed alcohol synthesis 2008 progress report. PNNL, Richland, WA
Gerber MA, White JF, Stevens DJ (2010) Mixed alcohol synthesis catalyst screening 2007 progress report. PNNL, Richland, WA
Subramani V, Gangwal SK (2008) Energy Fuels 22(2):814
Yoneda Y (1989) Progress in C1 Science in Japan. Amsterdam
Mei D, Rousseau R, Kathmann SM, Glezakou V-A, Engelhard MH, Jiang W, Wang C, Gerber MA, White JF, Stevens DJ (2010) J Catal 271(2):325
Eckle S, Anfang HG, Behm RJ (2011) J Phys Chem C 115(4):1361
Eckle S, Anfang HG, Behm RJ (2011) Appl Catal A Gen 391(1–2):325
Zhao YH, Sun KJ, Ma XF, Liu JX, Sun DP, Su HY, Li WX (2011) Angewandte Chemie-International Edition 50(23):5335
Choi Y, Liu P (2009) J Am Chem Soc 131(36):13054
Huo CF, Ren J, Li YW, Wang JG, Jiao HJ (2007) J Catal 249(2):174
Inderwildi OR, Jenkins SJ, King DA (2008) J Phys Chem C 112(5):1305
Ojeda M, Nabar R, Nilekar AU, Ishikawa A, Mavrikakis M, Iglesia E (2010) J Catal 272(2):287
Storsaeter S, Chen D, Holmen A (2006) Surf Sci 600(10):2051
CP2K, CP2K is a freely available program to perform atomistic and molecular simulations. http://cp2k.berlios.de
Perdew JP, Burke K, Ernzerhof M (1996) Phys Rev Lett 77(18):3865
Zhang YK, Yang WT (1998) Phys Rev Lett 80(4):890
Goedecker S, Teter M, Hutter J (1996) Phys Rev B 54(3):1703
VandeVondele J, Hutter J (2007) J Chem Phys 127(11):114105
Henkelman G, Uberuaga BP, Jonsson H (2000) J Chem Phys 113(22):9901
Lindemann F (1910) Z Phys 11:609
Acknowledgments
This work was supported by the U.S. Department of Energy (DOE), Office of Energy Efficiency and Renewable Energy Biomass Program. The Pacific Northwest National Laboratory (PNNL) is operated by Battelle for the DOE under Contract DE-AC05-76RL01830. A portion of the research was performed using EMSL, a national science user facility sponsored by the Department of Energy’s Office of Biological and Environmental Research located at PNNL.
Author information
Authors and Affiliations
Corresponding author
Electronic Supplementary Material
Below is the link to the electronic supplementary material.
Rights and permissions
About this article
Cite this article
Glezakou, VA., Jaffe, J.E., Rousseau, R. et al. The Role of Ir in Ternary Rh-Based Catalysts for Syngas Conversion to C2 + Oxygenates. Top Catal 55, 595–600 (2012). https://doi.org/10.1007/s11244-012-9836-9
Published:
Issue Date:
DOI: https://doi.org/10.1007/s11244-012-9836-9