Abstract
Five hundred ppm Pd/CeO2 catalyst was prepared and evaluated in selective hydrogenation of acetylene in large excess of ethylene since ceria has been recently found to be a reasonable stand-alone catalyst for this reaction. Pd/CeO2 catalyst could be activated in situ by the feed gas during reactions and the catalyst without reduction showed much better ethylene selectivity than the reduced one in the high temperature range due to the formation of oxygen vacancies by reduction. Excellent ethylene selectivity of ∼100% was obtained in the whole reaction temperature range of 50°C–200°C for samples calcined at temperatures of 600°C and 800°C. This could be ascribed to the formation of PdxCe1−xO2−y or Pd-O-Ce surface species based on the X-ray diffraction and X-ray photoelectron spectroscopy results, indicating the strong interaction between palladium and ceria.
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Borodzinki A. Selective hydrogenation of ethyne in ethene-rich streams on palladium catalysts. Part 1. Effect of changes to the catalyst during reaction. Catalysis Reviews. Science and Engineering, 2006, 48(2): 91–144
Azizi Y, Petit C, Pitchon V. Formation of polymer-grade ethylene by selective hydrogenation of acetylene over Au/CeO2 catalyst. Journal of Catalysis, 2008, 256(2): 338–344
Chesnokov V V, Podyacheva O Y, Richards R M. Influence of carbon nanomaterials on the properties of Pd/C catalysts in selective hydrogenation of acetylene. Materials Research Bulletin, 2017, 88: 78–84
McEwan L, Julius M, Roberts S, Fletcher J C Q. A review of the use of gold catalysts in selective hydrogenation reactions. Gold Bulletin, 2010, 43(4): 298–306
Pei G X, Liu X Y, Wang A, Lee A F, Isaacs M A, Li L, Pan X, Yang X, Wang X, Tai Z, et al. Ag alloyed Pd single-atom catalysts for efficient selective hydrogenation of acetylene to ethylene in excess ethylene. ACS Catalysis, 2015, 5(6): 3717–3725
Zhang S, Li J, Xia Z M, Wu C, Zhang Z Y, Ma Y Y, Qu Y Q. Towards highly active Pd/CeO2 for alkene hydrogenation by tuning Pd dispersion and surface properties of the catalysts. Nanoscale, 2017, 9(9): 3140–3149
Paier J, Penschke C, Sauer J. Oxygen defects and surface chemistry of ceria: Quantum chemical studies compared to experiment. Chemical Reviews, 2013, 113(6): 3949–3985
Hu Z, Liu X, Meng D, Guo Y, Guo Y, Lu G. Effect of ceria crystal plane on the physicochemical and catalytic properties of Pd/Ceria for CO and propane oxidation. ACS Catalysis, 2016, 6(4): 2265–2279
Atzori L, Cutrufello M G, Meloni D, Cannas C, Gazzoli D, Monaci R, Sini M F, Rombi E. Highly active NiO-CeO2 catalysts for synthetic natural gas production by CO2 methanation. Catalysis Today, 2018, 299: 183–192
Tan H Y, Wang J, Yu S Z, Zhou K B. Support morphology-dependent catalytic activity of Pd/CeO2 for formaldehyde oxidation. Environmental Science & Technology, 2015, 49(14): 8675–8682
Kang J H, Shin E W, Kim W J, Park J D, Moon S H. Selective hydrogenation of acetylene on Pd/SiO2 catalysts promoted with Ti, Nb and Ce oxides. Catalysis Today, 2000, 63(2–4): 183–188
Werner K, Weng X F, Calaza F, Sterrer M, Kropp T, Paier J, Sauer J, Wilde M, Fukutani K, Shaikhutdinov S, Freund H J. Toward an understanding of selective alkyne hydrogenation on ceria: On the impact of O vacancies on H2 interaction with CeO2(111). Journal of the American Chemical Society, 2017, 139(48): 17608–17616
Carrasco J, Vilé G, Fernández-Torre D, Pérez R, Pérez-Ramírez J, Ganduglia-Pirovano M V. Molecular-level understanding of CeO2 as a catalyst for partial alkyne hydrogenation. Journal of Physical Chemistry C, 2014, 118(10): 5352–5360
Vilé G, Bridier B, Wichert J, Pérez-Ramírez J. Ceria in hydrogenation catalysis: High selectivity in the conversion of alkynes to olefins. Angewandte Chemie International Edition, 2012, 51(34): 8620–8623
Nelson N C, Manzano J S, Sadow A D, Overbury S H, Slowing I I. Selective hydrogenation of phenol catalyzed by palladium on high-surface-area ceria at room temperature and ambient pressure. ACS Catalysis, 2015, 5(4): 2051–2061
Panagiotopoulou P, Kondarides D I. Effect of the nature of the support on the catalytic performance of noble metal catalysts for the water-gas shift reaction. Catalysis Today, 2006, 112(1–4): 49–52
Luo Y, Xiao Y, Cai G, Zheng Y, Wei K. Complete methanol oxidation in carbon monoxide streams over Pd/CeO2 catalysts: Correlation between activity and properties. Applied Catalysis B: Environmental, 2013, 136: 317–324
Boronin A I, Slavinskaya E M, Danilova I G, Gulyaev R V, Amosov Y I, Kuznetsov P A, Polukhina I A, Koscheev S V, Zaikovskii V I, Noskov A S. Investigation of palladium interaction with cerium oxide and its state in catalysts for low-temperature CO oxidation. Catalysis Today, 2009, 144(3): 201–211
Slavinskaya E M, Kardash T Y, Stonkus O A, Gulyaev R V, Lapin I N, Svetlichnyi V A, Boronin A I. Metal-support interaction in Pd/CeO2 model catalysts for CO oxidation: From pulsed laser-ablated nanoparticles to highly active state of the catalyst. Catalysis Science & Technology, 2016, 6(17): 6650–6666
Trovarelli A. Catalytic properties of ceria and CeO2-containing materials. Catalysis Reviews. Science and Engineering, 1996, 38(4): 439–520
Bera P, Patil K C, Jayaram V, Subbanna G N, Hegde M S. Ionic dispersion of Pt and Pd on CeO2 by combustion method: Effect of metal-ceria interaction on catalytic activities for NO reduction and CO and hydrocarbon oxidation. Journal of Catalysis, 2000, 196(2): 293–301
Yao H C, Yao Y F Y. Ceria in automotive exhaust catalysts. 1. Oxygen storage. Journal of Catalysis, 1984, 86(2): 254–265
Meunier F, Maffre M, Schuurman Y, Colussi S, Trovarelli A. Acetylene semi-hydrogenation over Pd-Zn/CeO2: Relevance of CO adsorption and methanation as descriptors of selectivity. Catalysis Communications, 2018, 105: 52–55
Padole M C, Gangwar B P, Pandey A, Singhal A, Sharma S, Deshpande P A. Adsorption of C2 gases over CeO2-based catalysts: Synergism of cationic sites and anionic vacancies. Physical Chemistry Chemical Physics, 2017, 19(21): 14148–14159
Zhang S, Chen C Y, Jang B W L, Zhu A M. Radio-frequency H2 plasma treatment of AuPd/TiO2 catalyst for selective hydrogenation of acetylene in excess ethylene. Catalysis Today, 2015, 256: 161–169
Zhu B, Jang B W L. Insights into surface properties of non-thermal RF plasmas treated Pd/TiO2 in acetylene hydrogenation. Journal of Molecular Catalysis A Chemical, 2014, 395: 137–144
Kurnatowska M, Kepinski L, Mista W. Structure evolution of nanocrystalline Ce1−xPdxO2−y mixed oxide in oxidizing and reducing atmosphere: Reduction-induced activity in low-temperature CO oxidation. Applied Catalysis B: Environmental, 2012, 117: 135–147
Guo T, Du J, Li J. The effects of ceria morphology on the properties of Pd/ceria catalyst for catalytic oxidation of low-concentration methane. Journal of Materials Science, 2016, 51(24): 10917–10925
Slavinskaya E M, Gulyaev R V, Zadesenets A V, Stonkus O A, Zaikovskii V I, Shubin Y V, Korenev S V, Boronin A I. Low-temperature CO oxidation by Pd/CeO2 catalysts synthesized using the coprecipitation method. Applied Catalysis B: Environmental, 2015, 166–167: 91–103
Spezzati G, Su Y, Hofmann J P, Benavidez A D, DeLaRiva A T, McCabe J, Datye A K, Hensen E J M. Atomically dispersed Pd O species on CeO2(111) as highly active sites for low-temperature CO oxidation. ACS Catalysis, 2017, 7(10): 6887–6891
Craciun R, Daniell W, Knözinger H. The effect of CeO2 structure on the activity of supported Pd catalysts used for methane steam reforming. Applied Catalysis A, General, 2002, 230(1): 153–168
Tessier D, Rakai A, Bozon-Verduraz F. Spectroscopic study of the interaction of carbon monoxide with cationic and metallic palladium in palladium-alumina catalysts. Journal of the Chemical Society, Faraday Transactions, 1992, 88(5): 741–749
Bensalem A, Verduraz F B. Palladium-ceria catalysts: Metal-support interactions and reactivity of palladium in selective hydrogenation of but-1-yne. Reaction Kinetics and Catalysis Letters, 1997, 60(1): 71–77
Vilé G, Wrabetz S, Floryan L, Schuster M E, Girgsdies F, Teschner D, Pérez-Ramírez J. Stereo- and chemoselective character of supported CeO2 catalysts for continuous-flow three-phase alkyne hydrogenation. ChemCatChem, 2014, 6(7): 1928–1934
Acknowledgements
This work is partially supported by Welch Foundation (#T-0014) and the CNMS user program of the Oak Ridge National Laboratory. Acknowledgment is made to the Donors of the American Chemical Society Petroleum Research Fund for partial support of this research, ACS PRF (#57596-UR5).
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Li, K., Lyu, T., He, J. et al. Selective hydrogenation of acetylene over Pd/CeO2. Front. Chem. Sci. Eng. 14, 929–936 (2020). https://doi.org/10.1007/s11705-019-1912-2
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DOI: https://doi.org/10.1007/s11705-019-1912-2