Selective hydrogenation of acetylene over Pd/CeO₂

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 Pd_xCe_1−xO_2−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.

Graphical abstract

Keywords

selective hydrogenation / acetylene / Pd/CeO₂ / strong interaction

References

[1] 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

[2] 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

[3] 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

[4] 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

[5] Pei G X, Liu X Y, Wang A, Lee A F, Isaacs M A, Li L, Pan X, Yang X, Wang X, Tai Z, . Ag alloyed Pd single-atom catalysts for efficient selective hydrogenation of acetylene to ethylene in excess ethylene. ACS Catalysis, 2015, 5(6): 3717–3725

[6] 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

[7] 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

[8] 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

[9] 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

[10] 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

[11] 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

[12] 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

[13] 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

[14] 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

[15] 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

[16] 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

[17] 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

[18] 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

[19] 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

[20] Trovarelli A. Catalytic properties of ceria and CeO₂-containing materials. Catalysis Reviews. Science and Engineering, 1996, 38(4): 439–520

[21] 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

[22] Yao H C, Yao Y F Y. Ceria in automotive exhaust catalysts. 1. Oxygen storage. Journal of Catalysis, 1984, 86(2): 254–265

[23] 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

[24] 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

[25] 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

[26] 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

[27] Kurnatowska M, Kepinski L, Mista W. Structure evolution of nanocrystalline Ce_1−xPd_xO_2−y mixed oxide in oxidizing and reducing atmosphere: Reduction-induced activity in low-temperature CO oxidation. Applied Catalysis B: Environmental, 2012, 117: 135–147

[28] 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

[29] 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

[30] 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

[31] 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

[32] 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

[33] 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

[34] 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

Acknowledgments

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).

RIGHTS & PERMISSIONS

2020 Higher Education Press and Springer-Verlag GmbH Germany, part of Springer Nature