Investigation of the preparation methodologies of Pd-Cu single atom alloy catalysts for selective hydrogenation of acetylene

doi:10.1007/s11705-015-1547-x

Front. Chem. Sci. Eng.

2015, Vol. 9

Issue (4) : 442-449 https://doi.org/10.1007/s11705-015-1547-x

RESEARCH ARTICLE

Investigation of the preparation methodologies of Pd-Cu single atom alloy catalysts for selective hydrogenation of acetylene

Xinxiang Cao,Arash Mirjalili,James Wheeler,Wentao Xie,Ben W.-L. Jang(

)

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

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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 single-atom 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.

Keywords H₂ pulse chemisorption palladium-copper bimetallic catalyst single atom alloy acetylene hydrogenation HAADF-STEM

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

Online First Date: 20 November 2015 Issue Date: 26 November 2015

Cite this article:

Xinxiang Cao,Arash Mirjalili,James Wheeler, et al. Investigation of the preparation methodologies of Pd-Cu single atom alloy catalysts for selective hydrogenation of acetylene[J]. Front. Chem. Sci. Eng., 2015, 9(4): 442-449.

URL:

https://academic.hep.com.cn/fcse/EN/10.1007/s11705-015-1547-x
https://academic.hep.com.cn/fcse/EN/Y2015/V9/I4/442

Fig.1 Sketch of (a) the ultrasonic reaction system to perform Pd/Cu galvanic replacement [18] and (b) the scheme for the three catalyst preparation methods: sequential impregnation, co-impregnation and galvanic replacement (GR)

Tab.1 Actual metal loadings, Cu : Pd atomic ratios and H₂ pulse chemisorption results of the resulted catalysts

Fig.2 H₂-TPR patterns of the catalysts of Cu_0.85, Cu_0.85Pd_0.03-seq, Cu_0.85Pd_0.03-co and Pd_0.03

Fig.3 HAADF-STEM images of (a) CuPd-GR and (b) Cu_0.85Pd_0.03-seq

Fig.4 (a) Conversion, (b) selectivity and (c) yield as a function of temperature for acetylene selective hydrogenation over Pd/γ-Al₂O₃ and bimetallic Pd-Cu/γ-Al₂O₃ catalysts

Fig.5 (a) Ethylene selectivity and (b) acetylene conversion with time for the acetylene selective hydrogenation at 125 °C over bimetallic Pd-Cu/γ-Al₂O₃ catalysts prepared by different methods

Fig.6 TGA weight loss results of the used bimetallic Pd-Cu/γ-Al₂O₃ catalysts prepared by different methods

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