Adsorption states of typical intermediates on Ag/Al2O3 catalyst mployed in the selective catalytic reduction of NOx by ethanol

doi:10.1016/S1872-2067(15)60873-7

Abstract

Abstract:

The adsorption of ethanol and important intermediates onto Ag/Al₂O₃ catalyst employed in the selective catalytic reduction of NO_x by ethanol was simulated by density functional theory. Considering the interaction between Ag metal and Al₂O₃support, typical Ag-O-Al entities, i.e., Ag-O-Al_tetra and Ag-O-Al_octa, (tetra = tetrahedral and octa = octahedral refer to the coordination sites of Al), were selected as potential adsorption sites on the surface of the catalyst. Ethanol, and enolic and isocyanate species were preferentially adsorbed and activated by Ag-O-Al_tetra entities rather than by Ag-O-Al_octa entities. The strong Lewis acidity of Al_tetra in the Ag-O-Al_tetra entity was very important, enabling the entity to accept an electron via forward donation from either the C-O σ bond in ethanol or the N-C σ bond in the -NCO species. Moreover, the hybridization of the Ag and Al orbitals was critical for electron back donation from the Ag-O-Al_tetra entity to the C-C π bond in the enolic species or N-C π bond in the -NCO species. The significant activation of the N-C bond in -NCO on the Ag-O-Al_tetra sites facilitated cleavage of -NCO to form N₂. Thus, we can conclude that the acidity of the Al site and the interaction between Ag and Al play key roles in the selective catalytic reduction of NO_x by ethanol over Ag/Al₂O₃.

Key words: Silver, Alumina, Nitrogen oxides, Selective catalytic reduction, Density functional theory

Hua Deng, Yunbo Yu, Hong He. Adsorption states of typical intermediates on Ag/Al₂O₃ catalyst mployed in the selective catalytic reduction of NO_x by ethanol[J]. Chinese Journal of Catalysis, 2015, 36(8): 1312-1320.

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https://www.cjcatal.com/EN/Y2015/V36/I8/1312

References

[1] Morin S, Savarino J, Frey M M, Yan N, Bekki S, Bottenheim J W, Martins J M F. Science, 2008, 322: 730
[2] He H, Ma Q X, Ma J Z, Zhang H X, Wang Y S, Ji D S, Tang G Q, Chu B W, Liu C, Hao J M. Sci Rep, 2014, 4: 4172
[3] Burch R, Breen J P, Meunier F C. Appl Catal B, 2002, 39: 283
[4] Shimizu K I, Satsuma A. Phys Chem Chem Phys, 2006, 8: 2677
[5] Liu Z M, Woo S I. Catal Rev Sci Eng, 2006, 48: 43
[6] He H, Zhang X L, Wu Q, Zhang C B, Yu Y B. Catal Surv Asia, 2008, 12: 38
[7] Granger P, Parvulescu V I. Chem Rev, 2011, 111: 3155
[8] Meunier F C, Ross J R H. Appl Catal B, 2000, 24: 23
[9] Bethke K A, Kung H H. J Catal, 1997, 172: 93
[10] He H, Zhang R D, Yu Y B, Liu J F. Chin J Catal (贺泓, 张润铎, 余运波, 刘俊峰. 催化学报), 2003, 24: 788
[11] Yu Y B, He H, Feng Q C. J Phys Chem B, 2003, 107: 13090
[12] She X, Flytzani-Stephanopoulos M. J Catal, 2006, 237: 79
[13] Zhang R D, Kaliaguine S. Appl Catal B, 2008, 78: 275
[14] Deng H, Yu Y B, Liu F D, Ma J Z, Zhang Y, He H. ACS Catal, 2014, 4: 2776
[15] Liu Z M, Ma L L, Junaid A S M. J Phys Chem C, 2010, 114: 4445
[16] Hu C H, Chizallet C, Mager-Maury C, Corral-Valerom M, Sautet P, Toulhoat H, Raybaud P. J Catal, 2010, 274: 99
[17] Digne M, Sautet P, Raybaud P, Euzen P, Toulhoat H. J Catal, 2002, 211: 1
[18] Digne M, Sautet P, Raybaud P, Euzen P, Toulhoat H. J Catal, 2004, 226: 54
[19] Lee J H, Yezerets A, Kung M C, Kung H H. Chem Commun, 2001: 404
[20] Yeom Y H, Li M J, Sachtler W M H, Weitz E. J Catal, 2006, 238: 100
[21] Tamm S, Ingelsten H H, Palmqvist A E C. J Catal, 2008, 255: 304
[22] Yu Y B, He H, Feng Q C, Gao H W, Yang X. Appl Catal B, 2004, 49: 159
[23] Yu Y B, Gao H W, He H. Catal Today, 2004, 93-95: 805
[24] He H, Yu Y B. Catal Today, 2005, 100: 37
[25] Satsuma A, Shimizu K I. Prog Energy Combus Sci, 2003, 29: 71
[26] Sumiya S, He H, Abe A, Takezawa N, Yoshida K. J Chem Soc Faraday Trans, 1998, 94: 2217
[27] Chansai S, Burch R, Hardacre C, Breen J, Meunier F. J Catal, 2010, 276: 49
[28] Chansai S, Burch R, Hardacre C, Breen J, Meunier F. J Catal, 2011, 281: 98
[29] Gao H W, He H. Spectrochim Acta A, 2005, 61: 1233
[30] Zhao S, Ren Y L, Wang J J, Yin W P. J Mol Struct: THEOCHEM, 2009, 897: 100
[31] He H, Li Y, Zhang X L, Yu Y B, Zhang C B. Appl Catal A, 2010, 375: 258
[32] Kim M K, Kim P S, Baik J H, Nam I S, Cho B K, Oh S H. Appl Catal B, 2011, 105: 1
[33] Breen J P, Burch R, Hardacre C, Hill C J. J Phys Chem B, 2005, 109: 4805
[34] Shimizu K I, Tsuzuki M, Kato K, Yokota S, Okumura K, Satsuma A. J Phys Chem C, 2007, 111: 950
[35] Korhonen S T, Beale A M, Newton M A, Weckhuysen B M. J Phys Chem C, 2011, 115: 885
[36] Yan Y, Yu Y B, He H, Zhao J J. J Catal, 2012, 293: 13
[37] Kwak J H, Hu J Z, Kim D H, Szanyi J S, Peden C H F. J Catal, 2007, 251: 189
[38] Kwak J H, Hu J Z, Lukaski A, Kim D H, Szanyi J S, Peden C H F. J Phys Chem C, 2008, 112: 9486
[39] Kwak J H, Mei D H, Yi C W, Kim D H, Peden C H F, Allard L F, Szanyi J. J Catal, 2009, 261: 17
[40] Kwak J H, Hu J Z, Mei D H, Yi C W, Kim D H, Peden C H F, Allard L F, Szanyi J. Science, 2009, 325: 1670
[41] Deng H, Yu Y B, He H. J Phys Chem C, 2015, 119: 3132
[42] Ukisu Y, Sato S, Muramatsu G, Yoshida K. Catal Lett, 1991, 11: 177
[43] Deng H, Yu Y B, He H. Catal Today, 2015, http://dx.doi.org/ 10.1016/j.cattod.2015.03.023
[44] Hoffman R. Rev Mod Phys, 1988, 60: 601
[45] Glassey W V, Hoffmann R. Surf Sci, 2001, 475: 47

Adsorption states of typical intermediates on Ag/Al₂O₃ catalyst mployed in the selective catalytic reduction of NO_x by ethanol

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