Abstract
The effects of Co loading and calcination temperatures on the catalytic activity of Co/Al2O3 for selective catalytic reduction (SCR) of NO with ethylene in excess oxygen were investigated. Co/Al2O3 showed high and low activities when calcined at high (800 °C) and low (350 °C) temperatures, respectively. The formation and dispersion of cobalt species for catalysts calcined at 350 and 800 °C as well as for Al2O3 were studied by XRD, UV–vis and FTIR spectra. Combined with DRIFTS results of ad-species and reaction experiments, it allowed us to correlate the catalytic activity with active sites of Co/Al2O3, and the catalytic functions of active cobalt species and support were clarified. Co3O4 species contributed to the oxidation of NO to various nitrates and of C2H4 to reactive formate species, even in the absence of O2, whereas the side reaction of ethylene combustion occurred simultaneously when excess oxygen was present. Tetrahedral Co2+ ions in CoAl2O4, which acted as the active sites, were responsible for the reaction between formate and nitrate species to form organic nitro compound.
Similar content being viewed by others
References
Liu Z, Woo SI (2006) Catal Rev Sci Eng 48:43
Amiridis MD, Mihut C, Maciejewski M, Baiker A (2004) Top Catal 28:141
Li Y, Armor JN (1992) Appl Catal B 1:L31
Armor JN, Farris TS (1994) Appl Catal B 4:L11
Burch R (2004) Catal Rev Sci Eng 46:271
Hamada H, Kintaichi Y, Yoshinari T, Tabata M, Sasaki M, Ito T (1993) Catal Today 17:111
Shimizu K, Maeshima H, Satsuma A, Hattori T (1998) Appl Catal B 18:163
Yan JY, Kung MC, Sachtler WMH, Kung HH (1997) J Catal 172:178
Lee JH, Schmieg SJ, Oh SH (2008) Appl Catal A 342:78
Takahashi M, Nakatani T, Iwamoto S, Watanabe T, Inoue M (2007) Appl Catal B 70:73
Hamada H, Kintaichi Y, Sasaki M, Ito T, Tabata M (1991) Appl Catal 75:L1
Li Y, Armor JN (1993) Appl Catal B 2:239
Maunula T, Ahola J, Hamada H (2000) Appl Catal B 26:173
He CH, Paulus M, Chu W, Find J, Nickl JA, Kohler K (2008) Catal Today 131:305
Nanba T, Uemura A, Ueno A, Haneda M, Hamada H, Kakuta N, Miura H, Ohfune H, Udagawa Y (1998) Bull Chem Soc Jpn 71:2331
Liotta LF, Pantaleo G, Macaluso A, Di Carlo G, Deganello G (2003) Appl Catal A 245:167
Hamada H (1994) Catal Today 22:21
Shimizu K, Shibata J, Yoshida H, Satsuma A, Hattori T (2001) Appl Catal B 30:151
Tavasoli A, Abbaslou RMM, Dalai AK (2008) Appl Catal A 346:58
Trepanier M, Tavasoli A, Dalai AK, Abatzoglou N (2009) Appl Catal A 353:193
Jacobs G, Patterson PM, Zhang Y, Das T, Li J, Davis BH (2002) Appl Catal A 233:215
Trigueiro FE, Ferreira CM, Volta JC, Gonzalez WA, Pries de Oliveria PG (2006) Catal Today 118:425
Brik Y, Kacimi M, Ziyad M, Verduraz FB (2001) J Catal 202:118
Gregorio FD, Bisson L, Armaroli T, Verdon C, Lemaitre L, Thomazeau C (2009) Appl Catal A 352:50
Jansson J (2000) J Catal 194:55
Finocchio E, Montanari T, Resini C, Busca G (2003) J Mol Catal A Chem 204–205:535
Arnoldy P, Moulijn JA (1985) J Catal 93:38
Shimizu K, Kawabata H, Maeshima H, Satsuma A, Hattori T (2000) J Phys Chem B 104:2885
Meunier FC, Breen JP, Zuzaniuk V, Olsson M, Ross JRH (1999) J Catal 187:493
Zhang XL, He H, Gao HW, Yu YB (2008) Spectrochim Acta Part A 71:1446
Meunier FC, Zuzaniuk V, Breen JP, Olsson M, Ross JRH (2000) Catal Today 59:287
Satsuma A, Shimizu K (2003) Prog Energy Combust Sci 29:71
Liu ZM, Woo SI, Lee WS (2006) J Phys Chem B 110:26019
He CH, Kohler K (2006) Phys Chem Chem Phys 8:898
Zuzaniuk V, Meunier FC, Ross JRH (2001) J Catal 202:340
Acknowledgments
The present work was supported by the National Natural Science Foundation of China (No.20573014 and 20077005) and by the Program for New Century Excellent Talents in University (NCET-07-0136), as well as by the National High Technology and Development Program (863 program) of China (Grant No.2007AA06Z311).
Author information
Authors and Affiliations
Corresponding author
Rights and permissions
About this article
Cite this article
Chen, X., Zhu, A. & Shi, C. The Nature of Active Sites of Co/Al2O3 for the Selective Catalytic Reduction of NO with C2H4 . Catal Lett 133, 134–141 (2009). https://doi.org/10.1007/s10562-009-0146-1
Received:
Revised:
Accepted:
Published:
Issue Date:
DOI: https://doi.org/10.1007/s10562-009-0146-1