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Enhanced stability of Pd/Al2O3 during aqueous oxidation reaction via SiH4 treatment

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Abstract

γ-Al2O3 is widely present as a support in catalytic application. However, the transformation of γ-Al2O3 into the undesired hydrated boehmite (γ-AlOOH) under the aqueous reaction conditions usually results in an irreversible inactivation of supported Al2O3 catalysts. Toward suppressing the hydration of γ-Al2O3 in the process of catalytic reactions, herein we have devised a new strategy by exploring the SiH4 treatment for successful preparation of Si–Pd/Al2O3 catalysts. SiH4 treatment enables a significant improvement in the poor stability of Pd/Al2O3 for selective oxidation of toluene because SiH4 could effectively anchor palladium nanoparticles and inhibit the formation of boehmite by reacting with unsaturated aluminum sites to reduce the intensity of Lewis acid sites on the surface of γ-Al2O3. Pd/Al2O3 pretreated with SiH4, that is Si–Pd/Al2O3, provides high catalytic activity and stability in the aqueous oxidation of toluene even at high temperature. Moreover, Si–Pd/Al2O3 is reusable without obvious loss of the catalytic activity and selectivity, compared to Pd/Al2O3.

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References

  1. Rinaldi R, Fujiwara FY, Schuchardt U (2006) Structural, morphological and acidic changes of nanocrystalline aluminas caused by a controlled humidity atmosphere. Appl Catal A 315:44–51

    Article  CAS  Google Scholar 

  2. Trueba M, Trasatti SP (2005) γ-alumina as a support for catalysts: a review of fundamental aspects. Eur J Inorg Chem 17:3393–3403

    Article  Google Scholar 

  3. Li H, Xu Y, Gao C, Zhao Y (2010) Structural and textural evolution of Ni/γ–Al2O3 catalyst under hydrothermal conditions. Catal Today 158:475–480

    Article  CAS  Google Scholar 

  4. Koichumanova K, Vikla AKK, Vlieger DJMD, S K, Mojet BL, Leon L (2013) Towards stable catalysts for aqueous phase conversion of ethylene glycol for renewable hydrogen. Chemsuschem 6:1717–1723

    Article  CAS  Google Scholar 

  5. Liang N, Zhang X, An H, Zhao X, Wang Y (2015) Direct synthesis of 2-ethylhexanol via n-butanal aldol condensation–hydrogenation reaction integration over a Ni/Ce–Al2O3 bifunctional catalyst. Green Chem 17:2959–2972

    Article  CAS  Google Scholar 

  6. Lefèvre G, Duc M, Lepeut P, Renaud Caplain A, Fédoroff M (2002) Hydration of γ-alumina in water and its effects on surface reactivity. Langmuir 18:7530–7537

    Article  Google Scholar 

  7. Ravenelle RM, Copeland JR, Kim WG, Crittenden JC, Sievers C (2011) Structural changes of γ-Al2O3-supported catalysts in hot liquid water. ACS Catal 1:552–561

    Article  CAS  Google Scholar 

  8. Jongerius AL, Copeland JR, Foo GS, Hofmann JP, Bruijnincx PCA, Sievers C, Weckhuysen BM (2013) Stability of Pt/γ–Al2O3 catalysts in lignin and lignin model compound solutions under liquid phase reforming reaction conditions. ACS Catal 3:464–473

    Article  CAS  Google Scholar 

  9. Parvulescu V, Constantin C, Su BL (2003) Liquid phase oxidation of aromatic hydrocarbons using highly ordered Nb and NbCo-MCM-41 nanoreactors. J Mol Catal A Chem 202:171–178

    Article  CAS  Google Scholar 

  10. Li L, Lv J, Shen Y, Guo X, Peng L, Xie Z, Ding W (2014) Hexadecylphosphate-functionalized iron oxide nanoparticles: mild oxidation of benzyl C–H bonds exclusive to carbonyls by molecular oxygen. ACS Catal 4:2746–2752

    Article  CAS  Google Scholar 

  11. Kesavan L, Tiruvalam R, Ab Rahim MH, bin Saiman MI, Enache DI, Jenkins RL, Dimitratos N, Lopez-Sanchez JA, Taylor SH, Knight DW (2011) Solvent-free oxidation of primary carbon–hydrogen bonds in toluene using Au–Pd alloy nanoparticles. Science 331:195–199

    Article  CAS  Google Scholar 

  12. Xiong H, Pham HN, Datye AK (2014) Hydrothermally stable heterogeneous catalysts for conversion of biorenewables. Green Chem 16:4627–4643

    Article  CAS  Google Scholar 

  13. Morterra C, Magnacca G (1996) A case study: surface chemistry and surface structure of catalytic aluminas, as studied by vibrational spectroscopy of adsorbed species. Catal Today 27:497–532

    Article  CAS  Google Scholar 

  14. Regali F, Liotta LF, Venezia AM, Montes V, Boutonnet M, Järås S (2014) Effect of metal loading on activity, selectivity and deactivation behavior of Pd/silica–alumina catalysts in the hydroconversion of n-hexadecane. Catal Today 223:87–96

    Article  CAS  Google Scholar 

  15. Gentile M, Xiao P, Abram T (2015) Palladium interaction with silicon carbide. J Nucl Mater 462:100–107

    Article  CAS  Google Scholar 

  16. Brown GE, Henrich VE, Casey WH, Clark DL, Eggleston C, Felmy A, Goodman DW, Grätzel M, Maciel G, McCarthy MI (1999) Metal oxide surfaces and their interactions with aqueous solutions and microbial organisms. Chem Rev 99:77–174

    Article  CAS  Google Scholar 

  17. Dong Z, Wang T, Zhao J, Fu T, Guo X, Peng L, Zhao B, Xue N, Ding W, Xie Z (2016) Ni-Silicides nanoparticles as substitute for noble metals for hydrogenation of nitrobenzene to p-Aminophenol in sulfuric acid. Appl Catal A 520:151–156

    Article  CAS  Google Scholar 

  18. Burtin P, Brunelle JP, Pijolat M, Soustelle M (1987) Influence of surface area and additives on the thermal stability of transition alumina catalyst supports. I: kinetic data. Appl Catal 34:225–238

    Article  CAS  Google Scholar 

  19. Ji H, Ling F, Wang S, Shen Z (2015) Relationship between surface acidity and microstructure of industrial γ-Al2O3. Pet Process Petrochem 46:17–21

    CAS  Google Scholar 

  20. Chin Y-H, Buda C, Neurock M, Iglesia E (2013) Consequences of metal–oxide interconversion for C–H bond activation during CH4 reactions on Pd catalysts. J Am Chem Soc 135:15425–15442

    Article  CAS  Google Scholar 

  21. Fu B, Zhu X, Xiao G (2012) Solvent-free selective aerobic oxidation of toluene by ultra fine nano-palladium catalyst. Appl Catal A 415–416:47–52

    Article  Google Scholar 

  22. Li S, Chen H, Wen M, Shen J (2016) Preparation of hydrothermally stable, basic, and highly active nano nickel catalysts for the hydrodeoxygenation of N, N-dimethylformamide. J Catal 338:1–11

    Article  CAS  Google Scholar 

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Acknowledgements

This work was financially supported by the Ministry of Science and Technology of China (2009CB623504), the National Science Foundation of China (20673054, 21273107, 21773109, 21503180) and Sinopec Shanghai Research Institute of Petrochemical Technology.

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Correspondence to Yan Zhu or Weiping Ding.

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Zhao, J., Dong, Z., Wang, T. et al. Enhanced stability of Pd/Al2O3 during aqueous oxidation reaction via SiH4 treatment. J Mater Sci 53, 15795–15803 (2018). https://doi.org/10.1007/s10853-018-2741-2

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  • DOI: https://doi.org/10.1007/s10853-018-2741-2

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