화학공학소재연구정보센터
Journal of Industrial and Engineering Chemistry, Vol.102, 103-111, October, 2021
Synthesis and characterization of Pd-Ni catalysts supported on KIT-6 and their application in cyclohexane oxidation using molecular oxygen
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Bimetallic Pd-Ni catalysts were prepared via impregnation method, with effects of Pd/Ni ratio (wt%) on their catalytic performance for the oxidation of cyclohexane with molecular oxygen being investigated. Synthesized catalysts were characterized by a series of techniques including XRD, Nitrogen adsorption- desorption, H2-TPR, XPS, ICP-AES, TEM, SEM, and EDX. Compared to monometallic Pd, the addition of Ni to Pd was found to be effective in enhancing the selective oxidation of cyclohexane. Parameters such as the temperature of the reaction, reaction times, catalyst amount, initial oxygen pressure and different solvents were investigated. Optimum conditions to improve cyclohexane conversion and selectivity towards KA-oil (a mixture of cyclohexanone and cyclohexanol) over 4.0%Pd-4.0%Ni/KIT-6 catalyst included 140 °C, 1.0 MPa O2 and acetonitrile as solvent. Under these reaction conditions, 10.87 % conversion and 95.45 % selectivity for KA-oil were observed after 8 h of reaction. Reusability studies of the selected catalyst revealed an outstanding stability along four reaction cycles.
  1. Li J, Shi Y, Xu L, Lu GZ, Ind. Eng. Chem. Res., 49(11), 5392 (2010)
  2. Zhao R, Wang Y, Guo Y, Guo Y, Liu X, Zhang Z, Wang Y, Zhan W, Lu G, Green Chem., 8, 459 (2006)
  3. Li J, Li X, Shi Y, Mao DS, Lu GZ, Catal. Lett., 137(3-4), 180 (2010)
  4. Martins LMDRS, Pombeiro AJL, Eur. J. Inorg. Chem., 2016, 2236 (2016)
  5. Du R, Yuan H, Yao J, Li H, AAPG Bull., 467, 24 (2019)
  6. Lu JQ, Zhang XM, Bravo-Suarez JJ, Tsubota S, Gaudet J, Oyama ST, Catal. Today, 123(1-4), 189 (2007)
  7. Nasrollahzadeh M, Nezafat Z, Bidgoli NSS, Shafiei N, Mol. Catal., 484 (2020)
  8. Huang XF, Yuan GF, Huang G, Wei SJ, J. Ind. Eng. Chem. (2019).
  9. Tan SJ, Ji YF, Zhao Y, Zhao AD, Wang B, Yang JL, Hou JG, J. Am. Chem. Soc., 133(6), 2002 (2011)
  10. Wittstock A, Zielasek V, Biener J, Friend CM, Baumer M, Science, 327(5963), 319 (2010)
  11. Zope BN, Hibbitts DD, Neurock M, Davis RJ, Science, 330(6000), 74 (2010)
  12. Yang W, Zhu Y, You F, Yan L, Ma Y, Lu C, Gao P, Hao Q, Li W, Appl. Catal. B: Environ., 223, 184 (2018)
  13. Ferrando R, Jellinek J, Johnston RL, Chem. Rev., 108(3), 845 (2008)
  14. Singh AK, Xu Q, ChemCatChem, 5, 652 (2013)
  15. Xu Y, Chen L, Wang X, Yao W, Zhang Q, Nanoscale, 7, 10559 (2015)
  16. Clarke JKA, Chem. Rev., 75, 291 (1975)
  17. Gao F, Goodman DW, Chem. Soc. Rev., 41, 8009 (2012)
  18. Tsubaki N, Sun SL, Fujimoto K, J. Catal., 199(2), 236 (2001)
  19. Yarulin A, Yuranov I, Cardenas-Lizana F, Alexander DTL, Kiwi-Minsker L, Appl. Catal. A: Gen., 478, 186 (2014)
  20. Goulas KA, Sreekumar S, Song Y, Kharidehal P, Gunbas G, Dietrich PJ, Johnson GR, Wang YC, Grippo AM, Grabow LC, Gokhale AA, Toste FD, J. Am. Chem. Soc., 138(21), 6805 (2016)
  21. Childers DJ, Schweitzer NM, Shahari SMK, Rioux RM, Miller JT, Meyer RJ, J. Catal., 318, 75 (2014)
  22. Armbruster M, Behrens M, Cinquini F, et al., ChemCatChem, 4, 1048 (2012)
  23. Freakley SJ, He Q, Harrhy JH, Lu L, Crole DA, Morgan DJ, Ntainjua EN, Edwards JK, Carley AF, Borisevich AY, Kiely CJ, Hutchings GJ, Science, 351(6276), 965 (2016)
  24. Komatsu T, Inaba K, Uezono T, Onda A, Yashima T, Appl. Catal. A: Gen., 251(2), 315 (2003)
  25. Rezaei M, Chermahini AN, Dabbagh HA, Chem. Eng. J., 314, 515 (2017)
  26. Adeleye AT, Akande AA, Odoh CK, Philip M, Fidelis TT, Amos PI, Banjoko OO, J. Ind. Eng. Chem., 96, 59 (2021)
  27. Che J, Hao M, Yi W, Kobayashi H, Zhou Y, Xiao L, Fan J, Cuihua Xuebao/Chinese J. Catal., 38, 1870 (2017).
  28. Zhang H, Jin M, Xia Y, Chem. Soc. Rev., 41, 8035 (2012)
  29. Zhang HJ, Watanabe T, Okumura M, Haruta M, Toshima N, Nat. Mater., 11(1), 49 (2012)
  30. Hutchings GJ, J. Chem. Soc. Dalt. Trans., 5523 (2008).
  31. Chen M, Kumar D, Yi CW, Goodman DW, Science, 310, 291 (2005)
  32. Gao F, Goodman DW, Chem. Soc. Rev., 41, 8009 (2012)
  33. Hutchings GJ, Kiely CJ, Accounts Chem. Res., 46, 1759 (2013)
  34. Shao MH, Sasaki K, Adzic RR, J. Am. Chem. Soc., 128(11), 3526 (2006)
  35. Shao MH, Shoemaker K, Peles A, Kaneko K, Protsailo L, J. Am. Chem. Soc., 132(27), 9253 (2010)
  36. Enache DI, Edwards JK, Landon P, Solsona-Espriu B, Carley AF, Herzing AA, Watanabe M, Kiely CJ, Knight DW, Hutchings GJ, Science, 311, 362 (2006)
  37. Kim TW, Kleitz F, Paul B, Ryoo R, J. Am. Chem. Soc., 127(20), 7601 (2005)
  38. Kishor R, Ghoshal AK, Microporous Mesoporous Mater., 242, 127 (2017)
  39. Sing KS, Pure Appl Chem., 57, 603 (1985).
  40. Liu Q, Li J, Zhao Z, Gao M, Kong L, Liu J, Wei Y, Catal. Sci. Technol., 6, 5927 (2016)
  41. Kim TW, Kleitz F, Paul B, Ryoo R, J. Am. Chem. Soc., 127(20), 7601 (2005)
  42. Konopny LW, Juan A, Damiani DE, Appl. Catal. B: Environ., 15(1-2), 115 (1998)
  43. Tonetto GM, Ferreira ML, Damiani DE, J. Mol. Catal. A-Chem., 193(1-2), 121 (2003)
  44. Shekar SC, Murthy JK, Rao PK, Rao KSR, J. Mol. Catal. A-Chem., 191(1), 45 (2003)
  45. Neri G, Musolino MG, Milone C, Pietropaolo D, Galvagno S, Appl. Catal. A: Gen., 208(1-2), 307 (2001)
  46. Du C, Chen M, Wang W, Yin G, ACS Appl. Mater. Interfaces, 3, 105 (2011)
  47. Zhao J, Sarkar A, Manthiram A, Electrochim. Acta, 55(5), 1756 (2010)
  48. Kim KS, Winograd N, Chem. Phys. Lett., 30, 91 (1975)
  49. Guo L, Bai J, Li C, Liang H, Sun W, Meng Q, Xu T, New J. Chem., 37, 4037 (2013)
  50. Wen Y, Potter OE, Sridhar T, Chem. Eng. Sci., 52(24), 4593 (1997)
  51. Schuchardt U, Cardoso D, Sercheli R, Pereira R, Da Cruz RS, Guerreiro MC, Mandelli D, Spinace E, Pires EL, Appl. Catal. A: Gen., 211, 1 (2001)
  52. Arends IWCE, Sheldon RA, Appl. Catal. A: Gen., 212, 175 (2001)
  53. Hermans I, Nguyen TL, Jacobs PA, Peeters J, ChemphysChem, 6, 637 (2005)
  54. Liu X, Conte M, Sankar M, He Q, Murphy DM, Morgan D, Jenkins RL, Knight D, Whiston K, Kiely CJ, Hutchings GJ, Appl. Catal. A: Gen., 504, 373 (2015)
  55. Conte M, Liu X, Murphy DM, Taylor SH, Whiston K, Hutchings GJ, Catal. Lett., 146(1), 126 (2016)