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

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.

Key words： copper; palladium; catalysts; acetylene; selective hydrogenation

Acknowledgments

The financial support of the National Natural Science Foundation of China (Grant No. 1263094), Welch Foundation (No. T-0014), Key Scientific and Technological Project of Henan province, China (No. 182102410072) and Shanxi International Cooperation Project (No. 201703D421037) are acknowledged. A portion of this research was conducted at the Center for Nanophase Materials Sciences, which is a DOE Office of Science User Facility.

References

1 Vignola E, Steinmann S N, Farra A A, Vandegehuchte B D, Curulla D, Sautet P. Evaluating the risk of C–C bond formation during selective hydrogenation of acetylene on palladium. ACS Catalysis, 2018, 8(3): 1662–1671

2 Hu M, Zhang J, Zhu W, Chen Z, Gao X, Du X, Wan J, Zhou K, Chen C, Li Y. 50 ppm of Pd dispersed on Ni(OH)₂ nanosheets catalyzing semi-hydrogenation of acetylene with high activity and selectivity. Nano Research, 2018, 11(2): 905–912

3 Pei G X, Liu X, Yang X, Zhang L, Wang A, Li L, Wang H, Wang X, Zhang T. Performance of Cu-alloyed Pd single-atom catalyst for semihydrogenation of acetylene under simulated front-end conditions. ACS Catalysis, 2017, 7(2): 1491–1500

4 McCue A J, Shepherd A M, Anderson J A. Optimisation of preparation method for Pd doped Cu/Al₂O₃ catalysts for selective acetylene hydrogenation. Catalysis Science & Technology, 2015, 5(5): 2880–2890

5 McCue A J, Baker R T, Anderson J A. Acetylene hydrogenation over structured Au-Pd catalysts. Faraday Discussions, 2016, 188: 499–523

6 Feng J, Liu Y, Yin M, He Y, Zhao J, Sun J, Li D. Preparation and structure-property relationships of supported trimetallic PdAuAg catalysts for the selective hydrogenation of acetylene. Journal of Catalysis, 2016, 344: 854–864

7 Liu Y, Zhao J, He Y, Feng J, Wu T, Li D. Highly efficient PdAg catalyst using a reducible Mg-Ti mixed oxide for selective hydrogenation of acetylene: Role of acidic and basic sites. Journal of Catalysis, 2017, 348: 135–145

8 Zhou H, Yang X, Li L, Liu X, Huang Y, Pan X, Wang A, Li J, Zhang T. PdZn intermetallic nanostructure with Pd-Zn-Pd ensembles for highly active and chemoselective semi-hydrogenation of acetylene. ACS Catalysis, 2016, 6(2): 1054–1061

9 Meuniera F, Maffrea M, Schuurmana Y, Colussib 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

10 Kruppe C M, Krooswyk J D, Trenary M. Selective hydrogenation of acetylene to ethylene in the presence of a carbonaceous surface layer on a Pd/Cu (111) single-atom alloy. ACS Catalysis, 2017, 7(12): 8042–8049

11 McCue A J, Guerrero-Ruiz A, Rodríguez-Ramos I, Anderson J A. Palladium sulphide—a highly selective catalyst for the gas phase hydrogenation of alkynes to alkenes. Journal of Catalysis, 2016, 340: 10–16

12 Hu M, Wang X. Effect of N₃-species on selective acetylene hydrogenation over Pd/SAC catalysts. Catalysis Today, 2016, 263: 98–104

13 McCue A J, McKenna F M, Anderson J A. Triphenylphosphine: A ligand for heterogeneous catalysis too? Selectivity enhancement in acetylene hydrogenation over modified Pd/TiO₂ catalyst. Catalysis Science & Technology, 2015, 5(4): 2449–2459

14 Kyriakou G, Boucher M B, Jewell A D, Lewis E A, Lawton T J, Baber A E, Tierney H L, Flytzani-Stephanopoulos M, Sykes E C H. Isolated metal atom geometries as a strategy for selective heterogeneous hydrogenations. Science, 2012, 335(6073): 1209–1212

15 Cao X, Ji Y, Luo Y. Dehydrogenation of propane to propylene by a Pd/Cu single-atom catalyst: Insight from first-principles calculations. Journal of Physical Chemistry C, 2015, 119(2): 1016–1023

16 Cao X, Fu Q, Luo Y. Catalytic activity of Pd-doped Cu nanoparticles for hydrogenation as a single-atom-alloy catalyst. Physical Chemistry Chemical Physics, 2014, 16(18): 8367–8375

17 Boucher M B, Zugic B, Cladaras G, Kammert J, Marcinkowski M D, Lawton T J, Sykes E C H, Flytzani-Stephanopoulos M. Single atom alloy surface analogs in Pd_0.18Cu₁₅ nanoparticles for selective hydrogenation reactions. Physical Chemistry Chemical Physics, 2013, 15(29): 12187–12196

18 Cao X, Mirjalili A, Wheeler J, Xie W, Jang B W L. Investigation of the preparation methodologies of Pd-Cu single atom alloy catalysts for selective hydrogenation of acetylene. Frontiers of Chemical Science & Engineering, 2015, 9(4): 442–449

19 Liu Y, He Y, Zhou D, Feng J, Li D. Catalytic performance of Pd-promoted Cu hydrotalcite-derived catalysts in partial hydrogenation of acetylene: Effect of Pd-Cu alloy formation. Catalysis Science & Technology, 2016, 6(9): 3027–3037

20 Li Y N, Jang B W L. Non-thermal RF plasma effects on surface properties of Pd/TiO₂ catalysts for selective hydrogenation of acetylene. Applied Catalysis A, General, 2011, 392(1-2): 173–179

21 Liu C J, Li M, Wang J, Zhou X, Guo Q, Yan J, Li Y. Plasma methods for preparing green catalysts: Current status and perspective. Chinese Journal of Catalysis, 2016, 37(3): 340–348

22 Dow W P, Wang Y, Huang T. TPR and XRD studies of yttria-doped ceria/g-alumina-supported copper oxide catalyst. Applied Catalysis A, General, 2000, 190(1-2): 25–34

23 Renuka N K, Shijina A V, Praveen A K, Aniz C U. Redox properties and catalytic activity of CuO/g-Al₂O₃ Meso phase. Journal of Colloid and Interface Science, 2014, 434: 195–200

24 Sagar G V, Rao P V R, Srikanth C S, Chary K V R. Dispersion and reactivity of copper catalysts supported on Al₂O₃-ZrO₂. Journal of Physical Chemistry B, 2006, 110(28): 13881–13888

25 Li Y, Jang B W L. Selective hydrogenation of acetylene over Pd/Al₂O₃ catalysts: Effect of non-thermal RF plasma preparation methodologies. Topics in Catalysis, 2017, 60(12-14): 1–12

26 Sa J, Arteaga G D, Daley R A, Bernardi J, Anderson J A. Factors influencing hydride formation in a Pd/TiO₂ Catalyst. Journal of Physical Chemistry B, 2006, 110(34): 17090–17095

27 Ryu S K, Lee W K, Park S J. Thermal decomposition of hydrated copper nitrate [Cu(NO₃)₂·3H₂O] on activated carbon fibers. Carbon letters, 2004, 5: 180–185

28 Wu C, Yuan W, Huang Y, Xia Y, Yang H, Wang H, Liu X. Conversion of xylose into furfural catalyzed by bifunctional acidic ionic liquid immobilized on the surface of magnetic g-Al₂O₃. Catalysis Letters, 2017, 147(4): 953–963

29 Chen C S, Lin J H, Lai T W. Low-temperature water gas shift reaction on Cu/SiO₂ prepared by an atomic layer epitaxy technique. Chemical Communications, 2008, 40(40): 4983–4985

30 Dulaurent O, Courtois X, Perrichon V, Bianchi D J. Heats of adsorption of CO on a Cu/Al₂O₃ catalyst using FTIR spectroscopy at high temperatures and under adsorption equilibrium conditions. Journal of Physical Chemistry B, 2000, 104(25): 6001–6011

31 Fernández-García M, Anderson J A, Haller G L. Alloy formation and stability in Pd-Cu bimetallic catalysts. Journal of Chemical Physics, 1996, 100(40): 16247–16254

32 Mierczynski P, Vasilev K, Mierczynsk A, Maniukiewicz W, Maniecki T P. Highly selective Pd-Cu/ZnAl₂O₄ catalyst for hydrogen production. Applied Catalysis A, General, 2014, 479(6): 26–34

33 McCue A J, Anderson J A. CO induced surface segregation as a means of improving surface composition and enhancing performance of CuPd bimetallic catalysts. Journal of Catalysis, 2016, 344: 854–864

34 Marakatti V S, Sarma S C, Joseph B, Banerjee D, Peter S C. Synthetically tuned atomic ordering in PdCu nanoparticles with enhanced catalytic activity towards solvent free benzylamine oxidation. ACS Applied Materials & Interfaces, 2017, 9(4): 3602–3615

35 Shao L D, Zhang W, Armbruster M, Teschner D, Girgsdies F, Zhang B S, Timpe O, Friedrich M, Schlogl R, Su D S. Nanosizing intermetallic compounds onto carbon nanotubes: Active and selective hydrogenation catalysts. Angewandte Chemie International Edition, 2011, 50(43): 10231–10235

36 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

37 Lee J W, Liu X, Mou C Y. Selective hydrogenation of acetylene over SBA-15 supported Au-Cu bimetallic catalysts. Journal of the Chinese Chemical Society (Taipei), 2013, 60(7): 907–914