Selective hydrogenation of acetylene over Pd/CeO<sub>2</sub>

doi:10.1007/s11705-019-1912-2

Front. Chem. Sci. Eng.

2020, Vol. 14

Issue (6) : 929-936 https://doi.org/10.1007/s11705-019-1912-2

RESEARCH ARTICLE

Selective hydrogenation of acetylene over Pd/CeO₂

Kai Li, Tengteng Lyu, Junyi He, Ben W. L. Jang(

)

Department of Chemistry, Texas A&M University Commerce, PO Box 3011, Commerce, TX 75429, USA

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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_xCe₁₋_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.

Keywords selective hydrogenation acetylene Pd/CeO₂ strong interaction

Corresponding Author(s): Ben W. L. Jang

Just Accepted Date: 13 February 2020 Online First Date: 20 March 2020 Issue Date: 11 September 2020

Cite this article:

Kai Li,Tengteng Lyu,Junyi He, et al. Selective hydrogenation of acetylene over Pd/CeO₂[J]. Front. Chem. Sci. Eng., 2020, 14(6): 929-936.

URL:

https://academic.hep.com.cn/fcse/EN/10.1007/s11705-019-1912-2
https://academic.hep.com.cn/fcse/EN/Y2020/V14/I6/929

Fig.1 Schematic diagram of the experimental setup.

Fig.2 H₂-TPR profiles of 500 ppm Pd/CeO₂.

Fig.3 XRD patterns for 500 ppm Pd/CeO₂ and commercial ceria.

Fig.4 (a) Pd 3d and (b) O 1s XPS spectra for 500 ppm Pd/CeO₂.

Fig.5 FTIR spectra after 5-min desorption on 500 ppm Pd/CeO₂ (a) without reduction and (b) reduced at 250°C.

Fig.6 FTIR adsorption spectra versus time on 500 ppm Pd/CeO₂ C450 without reduction.

Tab.1 Lattice parameter, Pd^d⁺ percentage, BET surface area and adsorbed hydrogen of Pd/CeO₂ catalysts

Fig.7 (a) Acetylene conversion and (b) ethylene selectivity over 500 ppm Pd/CeO₂ C450 without reduction, and reduced at 100°C and 250°C.

Fig.8 Effect of calcination temperature on (a) acetylene conversion and (b) ethylene selectivity over 500 ppm Pd/CeO₂ catalyst.

1	A Borodzinki. 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 https://doi.org/10.1080/01614940500364909
2	Y Azizi, C Petit, V Pitchon. Formation of polymer-grade ethylene by selective hydrogenation of acetylene over Au/CeO2 catalyst. Journal of Catalysis, 2008, 256(2): 338–344 https://doi.org/10.1016/j.jcat.2008.04.003
3	V V Chesnokov, O Y Podyacheva, R M Richards. Influence of carbon nanomaterials on the properties of Pd/C catalysts in selective hydrogenation of acetylene. Materials Research Bulletin, 2017, 88: 78–84 https://doi.org/10.1016/j.materresbull.2016.12.013
4	L McEwan, M Julius, S Roberts, J C Q Fletcher. A review of the use of gold catalysts in selective hydrogenation reactions. Gold Bulletin, 2010, 43(4): 298–306 https://doi.org/10.1007/BF03214999
5	G X Pei, X Y Liu, A Wang, A F Lee, M A Isaacs, L Li, X Pan, X Yang, X Wang, Z Tai, 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 https://doi.org/10.1021/acscatal.5b00700
6	S Zhang, J Li, Z M Xia, C Wu, Z Y Zhang, Y Y Ma, Y Q Qu. Towards highly active Pd/CeO2 for alkene hydrogenation by tuning Pd dispersion and surface properties of the catalysts. Nanoscale, 2017, 9(9): 3140–3149 https://doi.org/10.1039/C6NR09297G
7	J Paier, C Penschke, J Sauer. Oxygen defects and surface chemistry of ceria: Quantum chemical studies compared to experiment. Chemical Reviews, 2013, 113(6): 3949–3985 https://doi.org/10.1021/cr3004949
8	Z Hu, X Liu, D Meng, Y Guo, Y Guo, G Lu. 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 https://doi.org/10.1021/acscatal.5b02617
9	L Atzori, M G Cutrufello, D Meloni, C Cannas, D Gazzoli, R Monaci, M F Sini, E Rombi. Highly active NiO-CeO2 catalysts for synthetic natural gas production by CO2 methanation. Catalysis Today, 2018, 299: 183–192 https://doi.org/10.1016/j.cattod.2017.05.065
10	H Y Tan, J Wang, S Z Yu, K B Zhou. Support morphology-dependent catalytic activity of Pd/CeO2 for formaldehyde oxidation. Environmental Science & Technology, 2015, 49(14): 8675–8682 https://doi.org/10.1021/acs.est.5b01264
11	J H Kang, E W Shin, W J Kim, J D Park, S H Moon. Selective hydrogenation of acetylene on Pd/SiO2 catalysts promoted with Ti, Nb and Ce oxides. Catalysis Today, 2000, 63(2-4): 183–188 https://doi.org/10.1016/S0920-5861(00)00458-2
12	K Werner, X F Weng, F Calaza, M Sterrer, T Kropp, J Paier, J Sauer, M Wilde, K Fukutani, S Shaikhutdinov, H J Freund. 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 https://doi.org/10.1021/jacs.7b10021
13	J Carrasco, G Vilé, D Fernández-Torre, R Pérez, J Pérez-Ramírez, M V Ganduglia-Pirovano. Molecular-level understanding of CeO2 as a catalyst for partial alkyne hydrogenation. Journal of Physical Chemistry C, 2014, 118(10): 5352–5360 https://doi.org/10.1021/jp410478c
14	G Vilé, B Bridier, J Wichert, J Pérez-Ramírez. Ceria in hydrogenation catalysis: High selectivity in the conversion of alkynes to olefins. Angewandte Chemie International Edition, 2012, 51(34): 8620–8623 https://doi.org/10.1002/anie.201203675
15	N C Nelson, J S Manzano, A D Sadow, S H Overbury, I I Slowing. 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 https://doi.org/10.1021/cs502000j
16	P Panagiotopoulou, D I Kondarides. 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 https://doi.org/10.1016/j.cattod.2005.11.026
17	Y Luo, Y Xiao, G Cai, Y Zheng, K Wei. Complete methanol oxidation in carbon monoxide streams over Pd/CeO2 catalysts: Correlation between activity and properties. Applied Catalysis B: Environmental, 2013, 136: 317–324 https://doi.org/10.1016/j.apcatb.2013.02.020
18	A I Boronin, E M Slavinskaya, I G Danilova, R V Gulyaev, Y I Amosov, P A Kuznetsov, I A Polukhina, S V Koscheev, V I Zaikovskii, A S Noskov. Investigation of palladium interaction with cerium oxide and its state in catalysts for low-temperature CO oxidation. Catalysis Today, 2009, 144(3): 201–211 https://doi.org/10.1016/j.cattod.2009.01.035
19	E M Slavinskaya, T Y Kardash, O A Stonkus, R V Gulyaev, I N Lapin, V A Svetlichnyi, A I Boronin. 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 https://doi.org/10.1039/C6CY00319B
20	A Trovarelli. Catalytic properties of ceria and CeO2-containing materials. Catalysis Reviews. Science and Engineering, 1996, 38(4): 439–520 https://doi.org/10.1080/01614949608006464
21	P Bera, K C Patil, V Jayaram, G N Subbanna, M S Hegde. 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 https://doi.org/10.1006/jcat.2000.3048
22	H C Yao, Y F Y Yao. Ceria in automotive exhaust catalysts. 1. Oxygen storage. Journal of Catalysis, 1984, 86(2): 254–265 https://doi.org/10.1016/0021-9517(84)90371-3
23	F Meunier, M Maffre, Y Schuurman, S Colussi, A Trovarelli. Acetylene semi-hydrogenation over Pd-Zn/CeO2: Relevance of CO adsorption and methanation as descriptors of selectivity. Catalysis Communications, 2018, 105: 52–55 https://doi.org/10.1016/j.catcom.2017.11.012
24	M C Padole, B P Gangwar, A Pandey, A Singhal, S Sharma, P A Deshpande. Adsorption of C2 gases over CeO2-based catalysts: Synergism of cationic sites and anionic vacancies. Physical Chemistry Chemical Physics, 2017, 19(21): 14148–14159 https://doi.org/10.1039/C7CP01207A
25	S Zhang, C Y Chen, B W L Jang, A M Zhu. Radio-frequency H2 plasma treatment of AuPd/TiO2 catalyst for selective hydrogenation of acetylene in excess ethylene. Catalysis Today, 2015, 256: 161–169 https://doi.org/10.1016/j.cattod.2015.04.002
26	B Zhu, B W L Jang. 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 https://doi.org/10.1016/j.molcata.2014.08.015
27	M Kurnatowska, L Kepinski, W Mista. 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 https://doi.org/10.1016/j.apcatb.2011.12.034
28	T Guo, J Du, J Li. 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 https://doi.org/10.1007/s10853-016-0303-z
29	E M Slavinskaya, R V Gulyaev, A V Zadesenets, O A Stonkus, V I Zaikovskii, Y V Shubin, S V Korenev, A I Boronin. Low-temperature CO oxidation by Pd/CeO2 catalysts synthesized using the coprecipitation method. Applied Catalysis B: Environmental, 2015, 166–167: 91–103 https://doi.org/10.1016/j.apcatb.2014.11.015
30	G Spezzati, Y Su, J P Hofmann, A D Benavidez, A T DeLaRiva, J McCabe, A K Datye, E J M Hensen. Atomically dispersed Pd–O species on CeO2(111) as highly active sites for low-temperature CO oxidation. ACS Catalysis, 2017, 7(10): 6887–6891 https://doi.org/10.1021/acscatal.7b02001
31	R Craciun, W Daniell, H Knözinger. 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 https://doi.org/10.1016/S0926-860X(01)01003-1
32	D Tessier, A Rakai, F Bozon-Verduraz. 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 https://doi.org/10.1039/FT9928800741
33	A Bensalem, F B Verduraz. 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 https://doi.org/10.1007/BF02477692
34	G Vilé, S Wrabetz, L Floryan, M E Schuster, F Girgsdies, D Teschner, J Pérez-Ramírez. Stereo- and chemoselective character of supported CeO2 catalysts for continuous-flow three-phase alkyne hydrogenation. ChemCatChem, 2014, 6(7): 1928–1934 https://doi.org/10.1002/cctc.201402124

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