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Received July 1, 2017
Accepted September 25, 2017
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Effects of copper loading on NH3-SCR and NO oxidation over Cu impregnated CHA zeolite
1Materials Science and Chemical Engineering Department, Stony Brook University, Stony Brook, NY 11794, U.S.A., USA 2Geosciences Department, Stony Brook University, Brook, NY 11794, U.S.A., USA 3Center for Functional Laboratory, Brookhaven National Laboratory, Upton, NY 11973, U.S.A., USA
Korean Journal of Chemical Engineering, January 2018, 35(1), 89-98(10), 10.1007/s11814-017-0268-x
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Abstract
Cu/CHA catalysts with various Cu loadings (0.5 wt%-6.0 wt%) were synthesized via incipient wetness impregnation. The catalysts were applied to the selective catalytic reduction (SCR) of NO with NH3 and NO oxidation reaction. XRD and N2 adsorption-desorption data showed that CHA structure was maintained with the incorporation of Cu, while specific surface areas decreased with increasing Cu loading. At intermediate Cu loading, 4 wt%, the highest NH3-SCR activity was observed with ~98% N2 selectivity from 150 °C to 300 °C. Small amounts of water, 2%, slightly increased NO conversion in addition to the remarkable N2O and NO2 reduction at high temperature. Water effects are attributed to the improved Cu ion reducibility and mobility. NO oxidation results provided no relation between NO2 formation and SCR activity. Physicochemical properties, NO conversion, N2 selectivity, and activation energy data showed that impregnated samples’ molecular structure and catalytic activity are comparable to the conventional ion-exchanged (IE) samples’ ones.
Keywords
References
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Crutzen PJ, Bruhl C, J. Phys. Chem. A, 105(9), 1579 (2001)
Ravishankara AR, Chem. Rev., 103(12), 4505 (2003)
Fritz A, Pitchon V, Appl. Catal. B: Environ., 13(1), 1 (1997)
Li JH, Chang HZ, Ma L, Hao JM, Yang RT, Catal. Today, 175(1), 147 (2011)
Roy S, Hegde MS, Madras G, Appl. Energy, 86(11), 2283 (2009)
Gao F, Kwak JH, Szanyi J, Peden CHF, Top. Catal., 56, 1441 (2013)
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Busca G, Lietti L, Ramis G, Berti F, Appl. Catal. B: Environ., 18(1-2), 1 (1998)
Long RQ, Yang RT, J. Am. Chem. Soc., 121(23), 5595 (1999)
Rahkamaa-Tolonen K, Maunula T, Lomma M, Huuhtanen M, Keiski RL, Catal. Today, 100(3-4), 217 (2005)
Kwak JH, Tran D, Szanyi J, Peden CHF, Lee JH, Catal. Lett., 142(3), 295 (2012)
Kwak JH, Tran D, Burton SD, Szanyi J, Lee JH, Peden CHF, J. Catal., 287, 203 (2012)
Gao F, Walter ED, Karp EM, Luo JY, Tonkyn RG, Kwak JH, Szanyi J, Peden CHF, J. Catal., 300, 20 (2013)
Wang D, Zhang L, Li JH, Kamasamudram K, Epling WS, Catal. Today, 231, 64 (2014)
Wang D, Zhang L, Kamasamudram K, Epling WS, ACS Catal., 3, 871 (2013)
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Ma L, Cheng YS, Cavataio G, McCabe RW, Fu LX, Li JH, Chem. Eng. J., 225, 323 (2013)
Wang D, Jangjou Y, Liu Y, Sharma MK, Luo JY, Li JH, Kamasamudram K, Epling WS, Appl. Catal. B: Environ., 165, 438 (2015)
Leistner K, Mihai O, Wijayanti K, Kumar A, Kamasamudram K, Currier NW, Yezerets A, Olsson L, Catal. Today, 258, 49 (2015)
Ma L, Cheng Y, Cavataio G, McCabe RW, Fu L, Li J, Appl. Catal. B: Environ., 156-157, 428 (2014)
Petitto C, Delahay G, Top. Catal., 59, 895 (2016)
Kwak JH, Tonkyn RG, Kim DH, Szanyi J, Peden CHF, J. Catal., 275(2), 187 (2010)
Deka U, Juhin A, Eilertsen EA, Emerich H, Green MA, Korhonen ST, J. Phys. Chem., 116, 4809 (2012)
Kispersky VF, Kropf AJ, Ribeiro FH, Miller JT, Phys. Chem. Chem. Phys., 14, 2229 (2012)
Kieger S, Delahay G, Coq B, Neveu B, J. Catal., 183(2), 267 (1999)
Zhang R, Li Y, Zhen T, RSC Adv., 4, 52130 (2014)
International Zeolite Association. http://www.iza-online.org/ (accessed 19 Feb, 2016).
Gao F, Kwak JH, Szanyi J, Peden CHF, Top. Catal., 56, 1441 (2013)
Gomez-Cazalilla M, Merida-Robles JM, Gurbani A, Rodriguez-Castellon E, Jimenez-Lopez A, J. Solid State Chem., 180, 1130 (2007)
Brandenberger S, Krocher O, Tissler A, Althoff R, Ind. Eng. Chem. Res., 50(8), 4308 (2011)
Shishkin A, Carlsson PA, Harelind H, Skoglundh M, Top. Catal., 56, 567 (2013)
Wang L, Gaudet JR, Li W, Weng D, J. Catal., 306, 68 (2013)
Vennestrøm PNR, Katerinopoulou A, Tiruvalam RR, Kustov A, Moses PG, Concepcion P, Corma A, ACS Catal., 3, 2158 (2013)
Zamadics M, Chen X, Kevan L, J. Phys. Chem., 96, 5488 (1992)
Pereda-Ayo B, De La Torre U, Illan-Gomez MJ, Bueno-Lopez A, Gonzalez-Velasco JR, Appl. Catal. B: Environ., 147, 420 (2014)
Xue JJ, Wang XQ, Qi GS, Wang J, Shen MQ, Li W, J. Catal., 297, 56 (2013)
Kieger S, Delahay G, Coq B, Neveu B, J. Catal., 183(2), 267 (1999)
Delahay G, Coq B, Kieger S, Neveu B, Catal. Today, 54(4), 431 (1999)
Kamasamudram K, Henry C, Currier N, Yezerets A, SAE Int. J. Engines., 5, 688 (2012)
Bartley GJ, Sharp C, SAE Int. J. Engines., 5, 683 (2012)
Kamasamudram K, Yezerets A, Chen X, Currier N, Castagnola M, Chen HY, SAE Int. J. Engines., 4, 1810 (2011)
Gao F, Washton NM, Wang YL, Kollar M, Szanyi J, Peden CHF, J. Catal., 331, 25 (2015)
Kwak JH, Zhu H, Lee JH, Peden CHF, Szanyi J, Chem. Commun., 48, 4758 (2012)
Kwak JH, Varga T, Peden CHF, Gao F, Hanson JC, Szanyi J, J. Catal., 314, 83 (2014)
Wang J, Yu T, Wang XQ, Qi GS, Xue JJ, Shen MQ, Li W, Appl. Catal. B: Environ., 127, 137 (2012)
Wang L, Li W, Qi GS, Weng D, J. Catal., 289, 21 (2012)
Xue JJ, Wang XQ, Qi GS, Wang J, Shen MQ, Li W, J. Catal., 297, 56 (2013)
Brandenberger S, Krocher O, Tissler A, Althoff R, Catal. Rev.-Sci. Eng., 50(4), 492 (2008)
Devadas M, Krocher O, Elsener M, Wokaun A, Soger N, Pfeifer M, Demel Y, Mussmann L, Appl. Catal. B: Environ., 67(3-4), 187 (2006)
Delahay G, Valade D, Guzman-Vargas A, Coq B, Appl. Catal. B: Environ., 55(2), 149 (2005)
Huang HY, Long RQ, Yang RT, Appl. Catal. A: Gen., 235(1-2), 241 (2002)
Long RQ, Yang RT, J. Catal., 207(2), 224 (2002)
Gao F, Walter ED, Kollar M, Wang YL, Szanyi J, Peden CHF, J. Catal., 319, 1 (2014)
Verma AA, Bates SA, Anggara T, Paolucci C, Parekh AA, Kamasamudram K, Yezerets A, Miller JT, Delgass WN, Schneider WF, Ribeiro FH, J. Catal., 312, 179 (2014)
Long RQ, Yang RT, J. Catal., 196(1), 73 (2000)
McEwen JS, Anggara T, Schneider WF, Kispersky VF, Miller JT, Delgass WN, Ribeiro FH, Catal. Today, 184(1), 129 (2012)
Sjovall H, Blint RJ, Olsson L, Appl. Catal. B: Environ., 92(1-2), 138 (2009)
Wang TJ, Baek SW, Kwon HJ, Kim YJ, Nam IS, Cha MS, Yeo GK, Ind. Eng. Chem. Res., 50(5), 2850 (2011)
Pant A, Schmieg SJ, Ind. Eng. Chem. Res., 50(9), 5490 (2011)
Bond GC, Keane MA, Kral H, Lercher JA, Catal. Rev.-Sci. Eng., 42(3), 323 (2000)
Richter M, Bentrup U, Eckelt R, Schneider M, Pohl MM, Fricke R, Appl. Catal. B: Environ., 51(4), 261 (2004)
Colombo M, Nova I, Tronconi E, Catal. Today, 151(3-4), 223 (2010)
Metkar PS, Salazar N, Muncrief R, Balakotaiah V, Harold MP, Appl. Catal. B: Environ., 104(1-2), 110 (2011)
Beale AM, Gao F, Lezcano-Gonzalez I, Peden CHF, Szanyi J, Chem. Soc. Rev., 44, 7371 (2015)
Schreier M, Teren S, Belcher L, Regalbuto JR, Miller JT, Nanotechnology, 16, S582 (2005)
Zuo Y, Han L, Bao W, Chang L, Wang J, Xuebao C, Chinese J. Catal., 34, 1112 (2013)
Li Y, Deng J, Song W, Liu J, Zhao Z, Gao M, Wei Y, J. Phys. Chem., 120, 14669 (2016)
