Abstract
Galvanic replacement, co-impregnation and sequential impregnation have been employed to prepare Pd-Cu bimetallic catalysts with less than 1 wt-% Cu and ca. 0.03 wt-% Pd for selective hydrogenation of acetylene in excess ethylene. High angle annular dark field-scanning transmission electron microscopy (HAADF-STEM) and H2 chemisorption results confirmed that Pd-Cu singleatom alloy structures were constructed in all three bimetallic catalysts. Catalytic tests indicated that when the conversion of acetylene was above 99%, the selectivity of ethylene of these three single atom alloy catalysts was still more than 73%. Furthermore, the single atom alloy catalyst prepared by sequential incipient wetness impregnation was found to have the best stability among the three procedures used.
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Li Y N, Jang W L B. Non-thermal RF plasma effects on surface properties of Pd/TiO2 catalysts for selective hydrogenation of acetylene. Applied Catalysis A, General, 2011, 392(1–2): 173–179
McCue A J, Shepherd A M, Anderson J A. Optimisation of preparation method for Pd doped Cu/Al2O3 catalysts for selective acetylene hydrogenation. Catalysis Science & Technology, 2015, 5(5): 2880–2890
Spanjers C S, Sim R S, Sturgis N P, Kabius B, Rioux R M. In situ spectroscopic characterization of Ni1–x Znx/ZnO catalysts and their selectivity for acetylene semihydrogenation in excess ethylene. ACS Catalysis, 2015, 5(6): 3304–3315
Tierney H L, Baber A E, Sykes E C H. Atomic-scale imaging and electronic structure determination of catalytic sites on Pd/Cu near surface alloys. Journal of Physical Chemistry C, 2009, 113(17): 7246–7250
Zhang Y, Diao W, Williams C T, Monnier J R. Selective hydrogenation of acetylene in excess ethylene using Ag- and Au- Pd/SiO2 bimetallic catalysts prepared by electroless deposition. Applied Catalysis A, General, 2014, 469: 419–426
Chen B, Dingerdissen U, Krauter J G E, Lansink R H G J, Möbus K, Ostgard D J, Panster P, Riermeier T H, Seebald S, Tacke T, Trauthwein H. New developments in hydrogenation catalysis particularlyin synthesis of fine and intermediate chemicals. Applied Catalysis A, General, 2005, 280(1): 17–46
McCue A J, McRitchie C J, Shepherd A M, Anderson J A. Cu/Al2O3 catalysts modified with Pd for selective acetylene hydrogenation. Journal of Catalysis, 2014, 319: 127–135
Menezes W G, Altmann L, Zielasek V, Thiel K, Bäumer M. Evidence for geometric effects in neopentane conversion on PdAu catalysts. Journal of Catalysis, 2013, 300: 125–135
Childers D J, Schweitzer N M, Shahri S M K, Rioux R M, Miller J T, Meyer R J. Evidence for geometric effects in neopentane conversion on PdAu catalysts. Catalysis Science & Technology, 2014, 4(12): 4366–4377
Tierney H L, Baber A E, Kitchin J R, Sykes E C H. Hydrogen dissociation and spillover on individual isolated palladium atoms. Physical Review Letters, 2009, 103(24): 2461021–2461024
Tierney H L, Baber A E, Sykes E C H. Dynamics of thioether molecular rotors: Effects of surface interactions and chain flexibility. Journal of Physical Chemistry C, 2009, 113(17): 7246–7250
Kyriakou G, Boucher M B, Jewell A D, Lewis E A, Lawton T J, Baber A E, Tierney H L, Flytzani Stephanopoulos M, Sykes E C H. Isolated metal atom geometries as a strategy for selective heterogeneous hydrogenations. Science, 2012, 335(6073): 1209–1212
Boucher M B, Zugic B, Cladaras G, Kammert J, Marcinkowski M D, Lawton T J, Sykes E C H, Flytzani S M. Single atom alloy surface analogs in Pd0.18Cu15 nanoparticles for selective hydrogenation reactions. Physical Chemistry Chemical Physics, 2013, 15(29): 12187–12196
Cao X, Fu Q, Luo Y. Catalytic activity of Pd-doped Cu nanoparticles for hydrogenation as a single-atom-alloy catalyst. Physical Chemistry Chemical Physics, 2014, 16(18): 8367–8375
Cao X, Ji Y, Luo Y. Dehydrogenation of propane to propylene by a Pd/Cu single-atom catalyst: Insight from first-principles calculations. Journal of Physical Chemistry C, 2015, 119(2): 1016–1023
Pei G X, Liu X Y, Wang A, Li L, Huang Y, Zhang T, Lee J W, Jang W L B, Mou C. Promotional effect of Pd single atoms on Au nanoparticles supported on silica for the selective hydrogenation of acetylene in excess ethylene. New Journal of Chemistry, 2014, 38(5): 2043–2051
Pei G X, Liu X Y, Wang A, Lee A F, Isaacs M A, Li L, Pan X, Yang X, Wang X, Tai Z, Wilson K, Zhang T. Ag alloyed Pd single-atom catalysts for efficient selective hydrogenation of acetylene to ethylene in excess ethylene. ACS Catalysis, 2015, 5(6): 3717–3725
Sun Z, Masa J, Xia W, König D, Ludwig A, Li Z A, Farle M, Schuhmann W, Muhler M. Rapid and surfactant-free synthesis of bimetallic Pt-Cu nanoparticles simply via ultrasound-assisted redox replacement. ACS Catalysis, 2012, 2(8): 1647–1653
Batista J, Pintar A, Mandrino D, Jenko M, Martin V. XPS and TPR examinations of γ-alumina supported Pd-Cu catalysts. Applied Catalysis A, General, 2001, 206(1): 113–124
Hackett S F J, Brydson R M, Gass M H, Harvey I, Newman A D, Wilson K, Lee A F. High-activity, single site mesoporous Pd/Al2O3 catalysts for selective aerobic oxidation of allylic alcohols. Angewandte Chemie, 2007, 119(45): 8747–8750
Batista J, Pintar A, Gomilšek J P, Kodre A, Bornette F. On the structural characteristics of γ-alumina-supported Pd-Cu bimetallic catalysts. Applied Catalysis A, General, 2001, 217(1–2): 55–68
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Cao, X., Mirjalili, A., Wheeler, J. et al. Investigation of the preparation methodologies of Pd-Cu single atom alloy catalysts for selective hydrogenation of acetylene. Front. Chem. Sci. Eng. 9, 442–449 (2015). https://doi.org/10.1007/s11705-015-1547-x
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DOI: https://doi.org/10.1007/s11705-015-1547-x