Size-controlled Pd Nanoparticles Supported on α-Al2O3 as Heterogeneous Catalyst for Selective Hydrogenation of Acetylene

doi:10.1016/S1004-9541(14)60070-7

Chin.J.Chem.Eng. ›› 2014, Vol. 22 ›› Issue (5): 516-521.DOI: 10.1016/S1004-9541(14)60070-7

Previous Articles Next Articles

Size-controlled Pd Nanoparticles Supported on α-Al₂O₃ as Heterogeneous Catalyst for Selective Hydrogenation of Acetylene

ZHANG Huoli¹, YANG Yuanyi^1,2, DAI Wei², LU Shuliang², YU Haibo², JI Yuanyuan²

1 Department of Chemical Engineering, Beijing University of Chemical Technology, Beijing 100029, China ;
2 Sinopec Beijing Research Institute of Chemical Industry, Beijing 100013, China

Received:2012-10-29 Revised:2013-02-28 Online:2014-05-06 Published:2014-05-28
Supported by:
Supported by SINOPEC Beijing Research Institute of Chemical Industry (01-09ZS0440, 11-08ZS0442).

Size-controlled Pd Nanoparticles Supported on α-Al₂O₃ as Heterogeneous Catalyst for Selective Hydrogenation of Acetylene

张火利¹, 杨元一^1,2, 戴伟², 鲁树亮², 于海波², 吉媛媛²

1 Department of Chemical Engineering, Beijing University of Chemical Technology, Beijing 100029, China;
2 Sinopec Beijing Research Institute of Chemical Industry, Beijing 100013, China

通讯作者: DAI Wei,E-mail: daiw.bjhy@sinopec.com
基金资助:
Supported by SINOPEC Beijing Research Institute of Chemical Industry (01-09ZS0440, 11-08ZS0442).

Abstract

Abstract: Size-controlled Pd nanoparticles (PdNPs) were synthesized in aqueous solution, using sodium carboxymethyl cellulose as the stabilizer. Size-controlled PdNPs were supported on α-Al₂O₃ by the incipient wetness impregnation method. The PdNPs on α-Al₂O₃ support were in a narrow particle size distribution in the range of 1-6 nm. A series of PdNPs/α-Al₂O₃ catalysts were used for the selective hydrogenation of acetylene in ethylene-rich stream. The results show that PdNPs/α-Al₂O₃ catalyst with 0.03% (by mass) Pd loading is a very effective and stable catalyst. With promoter Ag added, ethylene selectivity is increased from 41.0% to 63.8% at 100℃. Comparing with conventional Pd-Ag/α-Al₂O₃ catalyst, PdNPs-Ag/α-Al₂O₃ catalyst has better catalytic performance in acetylene hydrogenation and shows good prospects for industrial application.

Key words: Pd nanoparticles, sodium carboxymethyl cellulose, acetylene hydrogenation

摘要： Size-controlled Pd nanoparticles (PdNPs) were synthesized in aqueous solution, using sodium carboxymethyl cellulose as the stabilizer. Size-controlled PdNPs were supported on α-Al₂O₃ by the incipient wetness impregnation method. The PdNPs on α-Al₂O₃ support were in a narrow particle size distribution in the range of 1-6 nm. A series of PdNPs/α-Al₂O₃ catalysts were used for the selective hydrogenation of acetylene in ethylene-rich stream. The results show that PdNPs/α-Al₂O₃ catalyst with 0.03% (by mass) Pd loading is a very effective and stable catalyst. With promoter Ag added, ethylene selectivity is increased from 41.0% to 63.8% at 100℃. Comparing with conventional Pd-Ag/α-Al₂O₃ catalyst, PdNPs-Ag/α-Al₂O₃ catalyst has better catalytic performance in acetylene hydrogenation and shows good prospects for industrial application.

关键词: Pd nanoparticles, sodium carboxymethyl cellulose, acetylene hydrogenation

ZHANG Huoli, YANG Yuanyi, DAI Wei, LU Shuliang, YU Haibo, JI Yuanyuan. Size-controlled Pd Nanoparticles Supported on α-Al₂O₃ as Heterogeneous Catalyst for Selective Hydrogenation of Acetylene[J]. Chin.J.Chem.Eng., 2014, 22(5): 516-521.

张火利, 杨元一, 戴伟, 鲁树亮, 于海波, 吉媛媛. Size-controlled Pd Nanoparticles Supported on α-Al₂O₃ as Heterogeneous Catalyst for Selective Hydrogenation of Acetylene[J]. Chinese Journal of Chemical Engineering, 2014, 22(5): 516-521.

References

1 Borodziński, A., Bond, G.C., "Selective hydrogenation of ethyne in ethene-rich streams on palladium catalysts. Part 1. Effect of changes to the catalyst during reaction", Catal. Rev., 48, 91-144 (2006).

2 Molnár, Á., Sárkány, A., Varga, M., "Recirculation hydrogenation of carbon-carbon multiple bonds: Chemo-, regio- and stereo-selectivity", J. Mol. Catal. A: Chem., 173, 185-221 (2001).

3 Kang, J.H., Shin, E.W., Kim, W.J., Park, J.D., Moon, S.H., "Selective hydrogenation of acetylene on TiO₂-added Pd catalysts", J. Catal., 208, 310-320 (2002).

4 Khan, N.A., Shaikhutdinov, S., Freund, H.J., "Acetylene and ethylene hydrogenation on alumina supported Pd-Ag model catalysts", Catal. Lett., 108, 159-164 (2006).

5 Lee, J.H., Kim, S.K., Ahn, I.Y., Kim, W.J., Moon, S.H., "Performance of Pd-Ag/Al₂O₃ catalysts prepared by the selective deposition of Ag onto Pd in acetylene hydrogenation", Catal. Commun., 12, 1251-1254 (2011).

6 Borodziński, A., Cybulski, A., "The kinetic model of hydrogenation of acetylene-ethylene mixtures over palladium surface covered by carbonaceous deposits", Appl. Catal. A: Gen., 198, 51-66 (2000).

7 Mei, D., Neurock, M., Smith, C.M., "Hydrogenation of acetylene- ethylene mixtures over Pd and Pd-Ag alloys: First-principles-based kinetic monte carlo simulations", J. Catal., 268, 181-195 (2009).

8 Komhom, S., Mekasuwandumrong, O., Praserthdam, P., Panpranot, J., "Improvement of Pd/Al₂O₃ catalyst performance in selective acetylene hydrogenation using mixed phases Al₂O₃ support ", Catal. Commun., 10, 86-91 (2008).

9 Bronstein, L.M., Shifrina, Z.B., "Dendrimers as encapsulating, stabilizing, or directing agents for inorganic nanoparticles", Chem. Rev., 111, 5301-5344 (2011).

10 Roucoux, A., Schulz, J., Patin, H., "Reduced transition metal colloids: A novel family of reusable catalysts?", Chem. Rev., 102, 3757-3778 (2011).

11 Li, Y., Boone, E., EI-Sayed, M.A., "Size effects of PVP-Pd nanoparticles on the catalytic Suzuki reactions in aqueous solution", Langmuir, 18, 4921-4925 (2002).

12 Esuni, K., Isono, R., Yoshimura, T., "Preparation of PAMAM- and PPI-metal (silver, platinum and palladium) nanocomposites and their catalytic activities for reduction of 4-Nitrophenol", Langmuir, 20, 237-243 (2004).

13 Nemamcha, A., Rehspringer, J., Khatmi, K., "Synthesis of palladium nanoparticles by sonochemical reduction of palladium(II) nitrate in aqueous solution", J. Phys. Chem. B, 110, 383-387 (2006).

14 Gallon, B.J., Kojima, R.W., Kaner, R.B., Diaconescu, P.L., "Palladium nanoparticles supported on polyaniline nanofibers as a semi-heterogeneous catalyst in water", Angew. Chem. Int. Ed., 46, 7251-7254 (2007).

15 Evangelisti, C., Panziera, N., D’Alessio, A., Bertinetti, L., Botavina, M., "New monodispersed palladium nanoparticles stabilized by poly-(N-vinyl-2-pyrrolidone): Preparation, structural study and catalytic properties", J. Catal., 272, 246-252 (2010).

16 Lu, J.C., Sutton, J., Roberts, C.B., "Synthesis and extraction of monodisperse sodium carboxymethylcellulose-stabilized platinum nanoparticles for the self-assembly of ordered arrays", J. Phys. Chem. C, 111, 11566-11576 (2007).

17 Chen, J., Wang, J., Zhang, X., Jin, Y.L., "Microwave-assisted green synthesis of silver nanoparticles by carboxymethyl cellulose sodium and silver nitrate", Mater. Chem. Phys., 108, 421-424 (2008).

18 Zhang, H.L., Yang, Y.Y., Dai, W., Yang, D., Lu, S.L., Ji, Y.Y., "An aqueous-phase catalytic process for the selective hydrogenation of acetylene with monodisperse water soluble palladium nanoparticles as catalyst", Catal. Sci. Technol., 2, 1319-1323 (2012).

19 Liu, J., "Advanced electron microscopy of metal-support interactions in supported metal catalysts", Chem. Cat. Chem., 3, 934-948 (2011).

20 Zhang, Q.W., Li, J., Liu, X.X., Zhu, Q.M., "Synergetic effect of Pd and Ag dispersed on Al₂O₃ in the selective hydrogenation of acetylene", Appl. Catal. A: Gen., 197, 221-228 (2000).

21 Zhang, Q., Dai, W., Mu, W., Yu, H.B., "Pd-Ag/Al₂O₃ and Pd/Al₂O₃ catalysts for selective hydrogenation of ethyne with in-situ DRIFTS", CIESC Journal, 62, 71-77 (2011).

22 Palazov, A., Kadinov, G., Bonev, C.H., Shopov, D., "Infrared spectroscopic study of the interaction between carbon monoxide and hydrogen on supported palladium", J. Catal., 74, 44-54 (1982)

Size-controlled Pd Nanoparticles Supported on α-Al₂O₃ as Heterogeneous Catalyst for Selective Hydrogenation of Acetylene

Size-controlled Pd Nanoparticles Supported on α-Al₂O₃ as Heterogeneous Catalyst for Selective Hydrogenation of Acetylene

PDF (PC)

Knowledge

Abstract

Cite this article

share this article

References

Related Articles 0

Recommended Articles

Metrics

Comments