The DOI matches its Crossref record; 17 of the 17 references it cites were found in a registry or an index.
Correlating Particle Size and Shape of Supported Ru/γ-Al2O3 Catalysts with NH3 Decomposition Activity
Abstract
While ammonia synthesis and decomposition on Ru are known to be structure-sensitive reactions, the effect of particle shape on controlling the particle size giving maximum turnover frequency (TOF) is not understood. By controlling the catalyst pretreatment conditions, we have varied the particle size and shape of supported Ru/gamma-Al(2)O(3) catalysts. The Ru particle shape was reconstructed by combining microscopy, chemisorption, and extended X-ray absorption fine structure (EXAFS) techniques. We show that the particle shape can change from a round one, for smaller particles, to an elongated, flat one, for larger particles, with suitable pretreatment. Density functional theory calculations suggest that the calcination most likely leads to planar structures. We show for the first time that the number of active (here B(5)) sites is highly dependent on particle shape and increases with particle size up to 7 nm for flat nanoparticles. The maximum TOF (based on total exposed Ru atoms) and number of active (B(5)) sites occur at approximately 7 nm for elongated nanoparticles compared to at approximately 1.8-3 nm for hemispherical nanoparticles. A complete, first-principles based microkinetic model is constructed that can quantitatively describe for the first time the effect of varying particle size and shape on Ru activity and provide further support of the characterization results. In very small nanoparticles, particle size polydispersity (due to the presence of larger particles) appears to be responsible for the observed activity.
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Cites
Density-functional exchange-energy approximation with correct asymptotic behavior
Becke, A. D. (1988) · Physical Review A · doi:10.1103/physreva.38.3098 · Cited by 53,711
Density-functional approximation for the correlation energy of the inhomogeneous electron gas
Perdew, J. P. (1986) · Physical Review B · doi:10.1103/physrevb.33.8822 · Cited by 18,777
Electronic structure calculations on workstation computers: The program system turbomole
Ahlrichs, R., Bär, M., Häser, M., Horn, H., & Kölmel, C. (1989) · Chemical Physics Letters · doi:10.1016/0009-2614(89)85118-8 · Cited by 8,433
Handbook of Heterogeneous Catalysis
(1997) · Wiley eBooks · doi:10.1002/9783527619474 · Cited by 2,387
Ammonia Synthesis from First-Principles Calculations
Honkala, K., Hellman, A., Remediakis, I. N., Logadottir, A., Carlsson, A., Dahl, S., Christensen, C. H., & Nørskov, J. K. (2005) · Science · doi:10.1126/science.1106435 · Cited by 1,336
Heterogeneous catalysis in industrial practice
Satterfield, C. N. (1991) · Medical Entomology and Zoology · Cited by 1,211
Role of Steps inN2Activation on Ru(0001)
Dahl, S., Logadottir, A., Egeberg, R. C., Larsen, J. H., Chorkendorff, I., Törnqvist, E., & Nørskov, J. K. (1999) · Physical Review Letters · doi:10.1103/physrevlett.83.1814 · Cited by 788
A View from the Inside: Complexity in the Atomic Scale Ordering of Supported Metal Nanoparticles
Frenkel, A. I., Hills, C. W., & Nuzzo, R. G. (2001) · The Journal of Physical Chemistry B · doi:10.1021/jp012769j · Cited by 650
Self-citationStructure sensitivity of supported ruthenium catalysts for ammonia synthesis
Jacobsen, C. J. H., Dahl, S., Hansen, P. L., Törnqvist, E., Jensen, L., Topsøe, H., Prip, D. V., Møenshaug, P. B., & Chorkendorff, I. (2000) · Journal of Molecular Catalysis A: Chemical · doi:10.1016/s1381-1169(00)00396-4 · Cited by 431
Rosowski, F., Hornung, A., Hinrichsen, O., Herein, D., Muhler, M., & Ertl, G. (1997) · Applied Catalysis A: General · doi:10.1016/s0926-860x(96)00304-3 · Cited by 330
Dissociative adsorption of N on ru(0001): A surface reaction totally dominated by steps
DAHL, S., TORNQVIST, E., & CHORKENDORFF, I. (2000) · Journal of Catalysis · doi:10.1006/jcat.2000.2858 · Cited by 225
RAROGPILECKA, W., MISKIEWICZ, E., SZMIGIEL, D., & KOWALCZYK, Z. (2005) · Journal of Catalysis · doi:10.1016/j.jcat.2004.12.005 · Cited by 194
Steady-state decomposition of ammonia on the ruthenium(001) surface
Tsai, W., & Weinberg, W. H. (1987) · The Journal of Physical Chemistry · doi:10.1021/j100304a034 · Cited by 173
Mhadeshwar, A. B., Kitchin, J. R., Barteau, M. A., & Vlachos, D. G. (2004) · Catalysis Letters · doi:10.1023/b:catl.0000029523.22277.e1 · Cited by 100
Self-citationAmmonia decomposition on (1 1 10) and (0 0 1) surfaces of ruthenium
Egawa, C., Nishida, T., Naito, S., & Tamaru, K. (1984) · Journal of the Chemical Society Faraday Transactions 1 Physical Chemistry in Condensed Phases · doi:10.1039/f19848001595 · Cited by 84
Shu, Y., Murillo, L. E., Bosco, J. P., Huang, W., Frenkel, A. I., & Chen, J. G. (2008) · Applied Catalysis A General · doi:10.1016/j.apcata.2008.01.024 · Cited by 72
Self-citationEffect of Ru loading and of Ru precursor in Ru/C catalysts for ammonia synthesis
Rossetti, I., & Forni, L. (2005) · Applied Catalysis A General · doi:10.1016/j.apcata.2004.12.024 · Cited by 61
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van Deelen, T. W., Hernández Mejía, C., & de Jong, K. P. (2019) · Nature Catalysis · doi:10.1038/s41929-019-0364-x · Cited by 2,349
Ammonia as a possible element in an energy infrastructure: catalysts for ammonia decomposition
Schüth, F., Palkovits, R., Schlögl, R., & Su, D. S. (2012) · Energy Environ. Sci. · doi:10.1039/c2ee02865d · Cited by 828
Review of the Decomposition of Ammonia to Generate Hydrogen
Lucentini, I., Garcia, X., Vendrell, X., & Llorca, J. (2021) · Industrial & Engineering Chemistry Research · doi:10.1021/acs.iecr.1c00843 · Cited by 687
Low-temperature ammonia decomposition catalysts for hydrogen generation
Mukherjee, S., Devaguptapu, S. V., Sviripa, A., Lund, C. R. F., & Wu, G. (2018) · Applied Catalysis B: Environmental · doi:10.1016/j.apcatb.2017.12.039 · Cited by 671
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Wan, Z., Tao, Y., Shao, J., Zhang, Y., & You, H. (2021) · Energy Conversion and Management · doi:10.1016/j.enconman.2020.113729 · Cited by 553
Metadata
- Authors
- Karim, A. M., Prasad, V., Mpourmpakis, G., Lonergan, W. W., Frenkel, A. I., Chen, J. G., & Vlachos, D. G.
- Venue
- Journal of the American Chemical Society
- Publisher
- American Chemical Society (ACS)
- Published
- 2009-08-10
- Volume
- 131
- Issue
- 34
- Pages
- 12230-12239
- ISSN
- 0002-7863 (ISSN-L)
- 1520-5126
- OpenAlex
- W2056823453
- Cited by
- 428
- References
- 17
- FWCI
- 4.45
- Type
- journal article
- Language
- en
- Open access
- closed
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