Highly efficient hydrotalcite supported palladium catalyst for hydrodechlorination of 1, 2, 4-tri chlorobenzene: Influence of Pd loading

Abstract

The influence of Pd loading was studied for the gas phase catalytic hydrodechlorination of 1,2,4-trichlorobenzene over Pd supported on Mg-Al mixed oxide support with Mg:Al ratio 2:1. The Mg-Al support was prepared from hydrotalcite precursor. A series of catalysts was prepared with different loadings of Pd (1–6 wt%) on Mg-Al mixed oxide support. The performance of catalytic material was evaluated at different temperatures ranging from 425–575K. The fresh and used catalysts were characterized with different analytical techniques such as BET surface area, X-ray diffraction studies, Temperature programmed reduction, X-ray photoelectron spectroscopy and CO-chemisorption studies. H2-Temperature programmed desorption studies was also performed to understand the metal-support interaction and suitable active sites. The 4wt% of Pd on Mg-Al mixed oxide catalyst showed the highest conversion and selectivity among all catalysts and maintained steady activity with 10 h of time-on-stream studies. The main reasons for high activity are suitable metal-support interactions, Pd particle size, high surface area, and high surface Pd atomic concentration.

Graphic abstract

The influence of Pd loading was studied for gas phase catalytic hydrodechlorination of 1,2,4-trichlorobenzene over Pd supported on Mg-Al mixed oxide support with Mg:Al ratio 2:1. The different Pd-loadings in catalyst was studied for hydrodechlorination. The 4wt% of Pd on Mg-Al mixed oxide catalyst showed the highest performance among all the catalysts.

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References

  1. 1.

    Hashimoto Y and Ayame A 2003 Low-temperature hydrodechlorination of chlorobenzenes on platinum-supported alumina catalysts Appl. Catal. A: Gen. 250 247

    CAS  Google Scholar 

  2. 2.

    Zwiernik M J, Quensen J F and Boyd S A 1998 FeSO4 amendments stimulate extensive anaerobic PCB dechlorination Environ. Sci. Tech. 32 3360

    CAS  Google Scholar 

  3. 3.

    Kuipers B, Cullen W R and Mohn W W 1999 Reductive Dechlorination of Nonachlorobiphenyls and Selected Octachlorobiphenyls by Microbial Enrichment Cultures Environ. Sci. Tech. 33 3579

    CAS  Google Scholar 

  4. 4.

    DeWeerd K A and Bedard D L 1999 Use of halogenated benzoates and other halogenated aromatic compounds to stimulate the microbial dechlorination of PCBs Environ. Sci. Tech. 33 2057

    CAS  Google Scholar 

  5. 5.

    Coq B, Ferrat G and Figueras F 1986 Conversion of chlorobenzene over palladium and rhodium catalysts of widely varying dispersion J. Catal. 101 434

    CAS  Google Scholar 

  6. 6.

    Kawakami K and Kusunoki K 1975 Selectivity in consecutive hydrogenation of chlorobenzene in liquid phase Kagaku Kogaku Ronbunshu 1 559

    Google Scholar 

  7. 7.

    Coq B, Tijani A, Dutartre R and Figuéras F 1993 Influence of support and metallic precursor on the hydrogenation of p-chloronitrobenzene over supported platinum catalysts J. Mol. Catal. 79 253

    CAS  Google Scholar 

  8. 8.

    Coq B, Cognion J M, Figueras F and Tournigant D 1993 Conversion under hydrogen of dichlorodifluoromethane over supported palladium catalysts J. Catal. 141 21

    CAS  Google Scholar 

  9. 9.

    Coq B, Tijani A and Figuéras F 1991 Particle size effect on the kinetics of p-chloronitrobenzene hydrogenation over platinum/alumina catalysts J. Mol. Catal. 68 331

    CAS  Google Scholar 

  10. 10.

    Coq B, Tijani A and Figuéras F 1992 Influence of alloying platinum for the hydrogenation of p-chloronitrobenzene over PtM/Al2O3 catalysts with M Sn, Pb, Ge, Al, Zn J. Mol. Catal. 71 317

    CAS  Google Scholar 

  11. 11.

    Coq B, Dutartre R, Figueras F and Tazi T 1990 Particle size, precursor, and support effects in the hydrogenolysis of alkanes over supported rhodium catalysts J. Catal. 122 438

    CAS  Google Scholar 

  12. 12.

    Coq B, Bittar A, Dutartre R and Figueras F 1990 Influence of the precursor and the support on the catalytic properties of ruthenium for alkane hydrogenolysis Appl. Catal. 60 33

    CAS  Google Scholar 

  13. 13.

    Gómez-Quero S, Cárdenas-Lizana F and Keane M A 2013 Unique selectivity in the hydrodechlorination of 2,4-dichlorophenol over hematite-supported Au J. Catal. 303 41

    Google Scholar 

  14. 14.

    Sun J, Han Y, Fu H, Wan H, Xu Z and Zheng S 2018 Selective hydrodechlorination of 1,2-dichloroethane catalyzed by trace Pd decorated Ag/Al2O3 catalysts prepared by galvanic replacement Appl. Surf. Sci. 428 703

    CAS  Google Scholar 

  15. 15.

    Klokov S V, Lokteva E S, Golubina E V, Chernavskii P A, Maslakov K I, Egorova T B, et al. 2019 Cobalt–carbon nanocomposite catalysts of gas-phase hydrodechlorination of chlorobenzene Appl. Surf. Sci. 463 395

    CAS  Google Scholar 

  16. 16.

    Wu Y, Gan L, Zhang S, Song H, Lu C, Li W, et al. 2018 Carbon-nanotube-doped Pd-Ni bimetallic three-dimensional electrode for electrocatalytic hydrodechlorination of 4-chlorophenol: Enhanced activity and stability J. Hazard. Mater. 356 17

    CAS  PubMed  Google Scholar 

  17. 17.

    Cesteros Y, Salagre P, Medina F and Sueiras J 1999 Effect of the alumina phase and its modification on Ni/Al2O3 catalysts for the hydrodechlorination of 1, 2, 4-trichlorobenzene Appl. Catal. B: Environ. 22 135

    CAS  Google Scholar 

  18. 18.

    Cesteros Y, Salagre P, Medina F and Sueiras J 2000 Synthesis and characterization of several Ni/NiAl2O4 catalysts active for the 1, 2, 4-trichlorobenzene hydrodechlorination Appl. Catal. B: Environ. 25 213

    CAS  Google Scholar 

  19. 19.

    Hashimoto Y, Uemichi Y and Ayame A 2005 Low-temperature hydrodechlorination mechanism of chlorobenzenes over platinum-supported and palladium-supported alumina catalysts Appl. Catal. A: Gen. 287 89

    CAS  Google Scholar 

  20. 20.

    Keane M A, Pina G and Tavoularis G 2004 The catalytic hydrodechlorination of mono-, di-and trichlorobenzenes over supported nickel Appl. Catal. B: Environ. 48 275

    CAS  Google Scholar 

  21. 21.

    Chary K V, Rao P V R and Vishwanathan V 2006 Synthesis and high performance of ceria supported nickel catalysts for hydrodechlorination reaction Catal. Comm. 7 974

    CAS  Google Scholar 

  22. 22.

    Ordóñez S, Díez F V and Sastre H 2001 Characterisation of the deactivation of platinum and palladium supported on activated carbon used as hydrodechlorination catalysts Appl. Catal. B: Environ. 31 113

    Google Scholar 

  23. 23.

    Ordóñez S, Sastre H and Dıez F 2001 Thermogravimetric determination of coke deposits on alumina-supported noble metal catalysts used as hydrodechlorination catalysts Thermochim. Acta 379 25

    Google Scholar 

  24. 24.

    Díaz E, Ordóñez S, Bueres R F, Asedegbega-Nieto E and Sastre H 2010 High-surface area graphites as supports for hydrodechlorination catalysts: Tuning support surface chemistry for an optimal performance Appl. Catal. B: Environ. 99 181

    Google Scholar 

  25. 25.

    Meshesha B, Chimentão R, Medina F, Sueiras J, Cesteros Y, Salagre P, et al. 2009 Catalytic hydrodechlorination of 1, 2, 4-trichlorobenzene over Pd/Mg (Al) O catalysts Appl. Catal. B: Environ. 87 70

    CAS  Google Scholar 

  26. 26.

    Cesteros Y, Salagre P, Medina F, Sueiras J, Tichit D and Coq B 2001 Hydrodechlorination of 1, 2, 4-trichlorobenzene on nickel-based catalysts prepared from several Ni/Mg/Al hydrotalcite-like precursors Appl. Catal. B: Environ. 32 25

    CAS  Google Scholar 

  27. 27.

    Podila S, Alhamed Y A, AlZahrani A A and Petrov L A 2015 Hydrogen production by ammonia decomposition using Co catalyst supported on Mg mixed oxide systems Int. J. Hydrogen Energ. 40 15411

    CAS  Google Scholar 

  28. 28.

    Sing K S 1985 Reporting physisorption data for gas/solid systems with special reference to the determination of surface area and porosity (Recommendations 1984) Pure Appl. Chem. 57 603

    CAS  Google Scholar 

  29. 29.

    Seetharamulu P, Kumar V S, Padmasri A, Raju B D and Rao K R 2007 A highly active nano-Ru catalyst supported on novel Mg-Al hydrotalcite precursor for the synthesis of ammonia J. Mol. Catal. A: Chem. 263 253

    CAS  Google Scholar 

  30. 30.

    Shin E-J, Spiller A, Tavoularis G and Keane M A 1999 Chlorine-nickel interactions in gas-phase catalytic hydrodechlorination: catalyst deactivation and the nature of reactive hydrogen Phys. Chem. Chem. Phys. 1 3173

    CAS  Google Scholar 

  31. 31.

    Konvalinka J and Scholten J 1977 Sorption and temperature-programmed desorption of hydrogen from palladium and from palladium on activated carbon J. Catal. 48 374

    CAS  Google Scholar 

  32. 32.

    Chen Y, Hwang C and Liaw C 1998 One-step synthesis of methyl isobutyl ketone from acetone with calcined Mg/Al hydrotalcite-supported palladium or nickel catalysts Appl. Catal. A: Gen. 169 207

    CAS  Google Scholar 

  33. 33.

    Park C, Menini C, Valverde J L and Keane M A 2002 Carbon–chlorine and carbon–bromine bond cleavage in the catalytic hydrodehalogenation of halogenated aromatics J. Catal. 211 451

    CAS  Google Scholar 

  34. 34.

    Anderson J, Foger K and Breakspere R 1979 Adsorption and temperature-programmed desorption of hydrogen with dispersed platinum and platinum-gold catalysts J. Catal. 57 458

    CAS  Google Scholar 

  35. 35.

    Ouchaib T, Moraweck B, Massardier J and Renouprez A 1990 Charcoal supported palladium and palladium-chromium catalysts: a comparison in the hydrogenation of dienes with silica supported metals Catal. Today 7 191

    CAS  Google Scholar 

  36. 36.

    Amorim C, Yuan G, Patterson P M and Keane M A 2005 Catalytic hydrodechlorination over Pd supported on amorphous and structured carbon J. Catal. 234 268

    CAS  Google Scholar 

  37. 37.

    Conner Jr W C and Falconer J L 1995 Spillover in heterogeneous catalysis Chem. Rev. 95 759

    CAS  Google Scholar 

  38. 38.

    Contescu C, Macovei D, Craiu C, Teodorescu C and Schwarz J A 1995 Thermal induced evolution of chlorine-containing precursors in impregnated Pd/Al2O3 catalysts Langmuir 11 2031

    CAS  Google Scholar 

  39. 39.

    Di Cosimo J, Dıez V, Xu M, Iglesia E and Apesteguıa C 1998 Structure and surface and catalytic properties of Mg-Al basic oxides J. Catal. 178 499

    Google Scholar 

  40. 40.

    Gopinath R, Rao K N, Prasad P S, Madhavendra S, Narayanan S and Vivekanandan G 2002 Hydrodechlorination of chlorobenzene on Nb2O5-supported Pd catalysts: influence of microwave irradiation during preparation on the stability of the catalyst J. Mol. Catal. A: Chem. 181 215

    CAS  Google Scholar 

  41. 41.

    Urbano F and Marinas J 2001 Hydrogenolysis of organohalogen compounds over palladium supported catalysts J. Mol. Catal. A: Chem. 173 329

    CAS  Google Scholar 

  42. 42.

    Jujjuri S, Ding E, Shore S G and Keane M A 2007 A characterization of Ln-Pd/SiO2 (Ln= La, Ce, Sm, Eu, Gd and Yb): Correlation of surface chemistry with hydrogenolysis activity J. Mol. Catal. A: Chem. 272 96

    CAS  Google Scholar 

  43. 43.

    Halligudi S, Devassay B M, Ghosh A and Ravikumar V 2002 Kinetic study of vapor phase hydrodechlorination of halons by Pd supported catalysts J. Mol. Catal. A: Chem. 184 175

    CAS  Google Scholar 

  44. 44.

    Juszczyk W, Malinowski A and Karpiński Z 1998 Hydrodechlorination of CCl2F2 (CFC-12) over γ-alumina supported palladium catalysts Appl. Catal. A: Gen. 166 311

    CAS  Google Scholar 

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Acknowledgements

The funding for this research was supported by Deanship of Scientific Research (DSR) of King Abdulaziz University, Jeddah, under the Grant No. (D-109-135-1439). The authors thank the DSR for technical and financial support.

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Correspondence to Arshid M Ali or Seetharamulu Podila.

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Ali, A.M., Podila, S., Daous, M.A. et al. Highly efficient hydrotalcite supported palladium catalyst for hydrodechlorination of 1, 2, 4-tri chlorobenzene: Influence of Pd loading. J Chem Sci 132, 39 (2020). https://doi.org/10.1007/s12039-020-1743-1

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Keywords

  • Chloro-organic compounds
  • Mg-Al mixed oxide
  • Metal-support interaction