Preparation and investigation of Pd doped Cu catalysts for selective hydrogenation of acetylene

doi:10.1007/s11705-019-1822-3

Front. Chem. Sci. Eng.

2020, Vol. 14

Issue (4) : 522-533 https://doi.org/10.1007/s11705-019-1822-3

RESEARCH ARTICLE

Preparation and investigation of Pd doped Cu catalysts for selective hydrogenation of acetylene

Xinxiang Cao^1,^2,³, Tengteng Lyu¹, Wentao Xie¹, Arash Mirjalili¹, Adelaide Bradicich¹, Ricky Huitema¹, Ben W.-L. Jang¹(

), Jong K. Keum⁴, Karren More⁴, Changjun Liu³, Xiaoliang Yan⁵

¹. Department of Chemistry, Texas A&M University-Commerce, Commerce, TX 75429-3011, USA
². Laboratory for Development & Application of Cold Plasma Technology, College of Chemistry and Chemical Engineering, Luoyang Normal University, Luoyang 471022, China
³. Collaborative Innovation Center of Chemical Science and Engineering, School of Chemical Engineering and Technology, Tianjin University, Tianjin 300072, China
⁴. Center for Nanophase Materials Sciences and Chemical Science Division, Oak Ridge National Laboratory, Oak Ridge, TN 37831, USA
⁵. College of Chemistry and Chemical Engineering, Taiyuan University of Technology, Taiyuan 030024, China

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Abstract

A series of PdCu bimetallic catalysts with low Cu and Pd loadings and different Cu: Pd atomic ratios were prepared by conventionally sequential impregnation (CSI) and modified sequential impregnation (MSI) of Cu and Pd for selective hydrogenation of acetylene. Characterization indicates that the supported copper (II) nitrate in the PdCu bimetallic catalysts prepared by MSI can be directly reduced to Cu metal particles due to the hydrogen spillover from Pd to Cu(NO₃)₂ crystals. In addition, for the catalysts prepared by MSI, Pd atoms can form PdCu alloy on the surface of metal particles, however, for the catalysts prepared by CSI, Pd tends to migrate and exist below the surface layer of Cu. Reaction results indicate that compared with CSI, the MSI method enables samples to possess preferable stability as well as comparable reaction activity. This should be due to the MSI method in favor of the formation of PdCu alloy on the surface of metal particles. Moreover, even Pd loading is super low, <0.045 wt-% in this study, by through adjusting Cu loading to an appropriate value, attractive reactivity and selectivity still can be achieved.

Keywords copper palladium catalysts acetylene selective hydrogenation

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

Just Accepted Date: 04 April 2019 Online First Date: 18 June 2019 Issue Date: 22 May 2020

Cite this article:

Xinxiang Cao,Tengteng Lyu,Wentao Xie, et al. Preparation and investigation of Pd doped Cu catalysts for selective hydrogenation of acetylene[J]. Front. Chem. Sci. Eng., 2020, 14(4): 522-533.

URL:

https://academic.hep.com.cn/fcse/EN/10.1007/s11705-019-1822-3
https://academic.hep.com.cn/fcse/EN/Y2020/V14/I4/522

Tab.1 Metal loadings and Cu:Pd ratios of as-prepared catalysts

Fig.1 H₂-TPR patterns of as prepared fresh samples

Fig.2 (a) In situ XRD profiles of Cu₁₂-vac and (b) Pd_0.24Cu₁₂-vac in 4 vol-% H₂/He flow at different temperatures

Fig.3 CO-DRIFTs spectra of reduced samples, Cu_2.5-vac, Pd_0.05Cu_2.5-vac, Pd_0.05Cu_2.5-cal and Pd_0.05-cal

Fig.4 High-angle annular dark field (HAADF) STEM images of (a) Cu_2.5-vac, (b) Pd_0.05Cu_2.5-cal and (c) Pd_0.05Cu_2.5-vac and their corresponding lattice fringe (d), (e) and (f), respectively; STEM–EDS elemental maps (g, h and i) of a random particle in Pd_0.05Cu_2.5-vac

Fig.5 (a) Acetylene conversion and (b) selectivity to ethylene versus reaction temperature and the selectivity vs. the conversion over Pd_0.05-cal, Pd_0.05Cu_0.5-cal, Pd_0.05Cu_2.5-cal and Pd_0.05Cu_2.5-vac. H₂:C₂H₂:C₂H₄ = 3:1:99, GHSV= 60000 cc?g^–1?h^–1

Fig.6 (a) Acetylene conversion and (b) selectivity to ethylene versus reaction time over Pd_0.05Cu_2.5-cal and Pd_0.05Cu_2.5-vac. H₂:C₂H₂:C₂H₄ = 3:1:99, GHSV= 60000 cc?g^–1?h^–1, reaction temperature: 120°C

Fig.7 (a) TG results of fresh and used Pd_0.05Cu_2.5-cal and Pd_0.05Cu_2.5-vac and (b) corresponding DTG results of the two used samples derived from TG

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