Hydrogenolysis of nitrosodimethyl amine in gas phase over Au/γ-Al2O3 nanocatalyst

Shahram Ghanbari Pakdehi; Fariba Fazeli

Korean Journal of Chemical Engineering, Vol.31, No.7, 1174-1179, July, 2014

DOI10.1007/s11814-014-0024-4 Export Citation

Hydrogenolysis of nitrosodimethyl amine in gas phase over Au/γ-Al2O3 nanocatalyst

Shahram Ghanbari Pakdehi^†, and Fariba Fazeli¹

Faculty Chemical Engineering, Malek Ashtar University of Technology, P. O. Box 11365-8486, Tehran, Iran
¹Space Transportation Research Institute, Iranian Space Research Center, P. O. Box 13445-754, Tehran, Iran

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Nitrosodimethyl amine (NDMA), as a carcinogenic byproduct in production of unsymmetrical dimethyl hydrazine (UDMH) in space industries, should be decomposed in the vapor phase. A suitable method for this purpose is selective catalytic hydrogenolysis of NDMA over Au/γ-Al2O3 nanocatalyst. We synthesized and characterized the Au/γ-Al2O3 nanocatalyst by homogeneous deposition-precipitation (HDP)/DP-urea method. Activity of the catalyst was influenced by nanosized Au particles, Au loading and the bed temperature. The optimum parameters for the catalyst were: Au particles <5 nm, Au loading at 1.5 wt% and bed temperature of 35-45 ℃. The reaction was strongly sensitive to the Au particle size. The reaction occurred over the catalyst to produce dimethyl amine (DMA) and nitroxyl in a selective manner. The kinetics of NDMA hydrogenolysis over the nanocatalyst was studied in an integral fixed bed reactor. There existed a consistency with the Langmuir-Hinshelwood mechanism involving dissociative adsorption of H2 and NDMA.

Keywords:NDMA Hydrogenolysis;Au/γ-Al2O3 Nanocatalyst;Effective Parameters;Au Particle Size;Kinetics

[References]

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[1] Schmidt EW, Hydrazine and its derivatives (2nd Ed.), Wiley, New York (2001)

[2] Xu H, N-Nitrosamines in the environment, Science Press, Beijing (1988)

[3] Xu BB, Chen ZL, Qi F, Ma J, Wu FC, J. Hazard. Mater., 168(1), 108 (2009)

[4] Lee J, Choi W, Yon J, Environ. Sci. Technol., 39, 6800 (2005)

[5] Sharma VK, Sep. Purif. Technol., 88, 1 (2012)

[6] Gui L, Gillham RW, Odziemkowski MS, Environ. Sci. Technol., 34, 3489 (2000)

[7] Davie MG, Reinhard M, Shapley JR, Environ. Sci. Technol., 40, 7329 (2006)

[8] Smith GV, Notheisz F, Heterogeneous catalysis in organic chemistry, Academic Press, New York (1999)

[9] Haruta M, Catal. Surv. Jpn., 1, 61 (1997)

[10] Santos LL, Serna P, Corma A, Chem. Eur. J., 15, 8196 (2009)

[11] Corma A, Serna P, Science, 313, 332 (2006)

[12] Pakdehi SG, Sohrabi M, Chem. Eng. Technol., 34(11), 1840 (2011)

[13] Hugon A, Delannoy L, Krafft JM, Louis C, J. Phys. Chem. C, 114, 10823 (2010)

[14] Shiva S, Crawford JH, Ramachandran A, Ceaser EK, Hillson T, Brookes PS, Patel RP, Darley-Usmar VM, Biochem. J., 379, 359 (2004)

[15] Shafirovich V, Lymar SV, Proceedings of the National Academy of Sciences, 99, 7340 (2002)

[16] Greenwood NN, Earnshaw A, Chemistry of the elements, Elsevier, Oxford (1997)

[17] Kartusch C, van Bokhoven JA, Gold Bull., 42, 343 (2009)

[18] Bond GC, Thompson DT, Catal. Rev.-Sci. Eng., 41(3-4), 319 (1999)

[19] McEwana L, Juliusa M, Robertsa S, Fletchera JCQ, Gold Bull., 43, 298 (2010)

[20] Hussain A, A computational study of catalysis by gold in applications of CO oxidation, Ph.D. Thesis, Eindhoven: Technische Universiteit Eindhoven (2010)

[21] Comotti M, Nano-design as a powerful tool in gold catalyzed oxidation reactions, Ph.D. Thesis, Bochum: Universitat Bochum (2007)

[22] Okumura M, Akita T, Haruta M, Catal. Today, 74(3-4), 265 (2002)

[23] Huang D, Liao F, Molesa S, Redinger D, Subramanian V, J. Electrochem. Soc., 150, 412 (2003)

[24] Perego C, Peratello S, Catal. Today, 52(2-3), 133 (1999)

[25] Ishida T, Kawakita N, Akita T, Haruta M, Gold Bull., 42, 267 (2009)

[26] Aufray M, Roche AA, Appl. Surf. Sci., 254, 1936 (2007)