Fe-doped LaCoO3 perovskite catalyst for NO oxidation in the post-treatment of marine diesel engine’s exhaust emissions

So Ra An; Kyoung Ho Song; Kwan Young Lee; Ki Tae Park; Soon Kwan Jeong; Hak Joo Kim

Korean Journal of Chemical Engineering, Vol.35, No.9, 1807-1814, September, 2018

DOI10.1007/s11814-018-0097-6 Export Citation

Fe-doped LaCoO3 perovskite catalyst for NO oxidation in the post-treatment of marine diesel engine’s exhaust emissions

So Ra An^{1, 2}, Kyoung Ho Song^{1, 2}, Kwan Young Lee², Ki Tae Park¹, Soon Kwan Jeong¹, and Hak Joo Kim^{1, †}

¹Greenhouse Gas Research Laboratory, Korea Institute of Energy Research, Daejeon 34129, Korea
²Department of Chemical and Biological Engineering, Korea University, Seoul 02841, Korea

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New post-treatment process for marine diesel engine exhaust emissions was proposed by combining NO oxidation and wet scrubbing technology for the simultaneous removal of SOX, NOX and PM. NO, insoluble in aqueous scrubbing absorbent, is preferentially oxidized to NO2, which then turns fully soluble in it. Fe substituted LaCo1-xFexO3 perovskite catalysts were developed for NO oxidation to NO2. The catalysts were prepared by co-precipitation method and analyzed with XRD, XRF, BET, FT-IR, NO-TPD and XPS techniques. Crystal structure change from rhombohedral to orthorhombic was observed with the increased amount of Fe substituted in the B site of the perovskite by XRD analysis. From FT-IR and NO-TPD analysis, nitrate on perovskite species was found to be the active species for NO oxidation. Quantitative analysis was performed within the prepared catalysts. Catalytic activity was measured using a packed bed reactor operated at 150-400 °C, atmospheric pressure and with gas hourly space velocity (GHSV) of 20,000 h-1 using a simulated exhaust gas composed of NO 400 ppm, O2 10% balanced with N2. Formation of Fe4+ cation enhanced the redox property as well as the mobility of the lattice oxygen present in the perovskite catalysts, confirmed by XPS analysis. Reaction mechanism of NO oxidation on Fe substituted LaCo1-xFexO3 was discussed based on Mars-van Krevelen mechanism.

Keywords:Marine Exhaust Gas;NO Oxidation;Diesel Oxidation Catalyst (DOC);Perovskite Catalyst;Oxygen Vacancy;Mono- & Bi-dentate NO Adsorption;Fourier Transform-infrared Spectroscopy (FT-IR)

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[1] Wan Z, Zhu M, Chen S, Sperling D, Nature, 530(7590), 275 (2016)

[2] Ministry of Environment Republic of Korea, Environmental Statistics Yearbook in 2002. http://eng.me.go.kr/eng/web/main.do/, 2017 (Accessed 4 March 2017).

[3] Eide MS, Dalsøren SB, Endresen O, Samset B, Myhre G, Fuglestved J, Berntsen T, Atmos. Chem. Phys., 13, 4183 (2013)

[4] Dieselnet, International: IMO Marine Engine Regulations, http://www.dieselnet.com/standards/inter/imo.php/2017 (Accessed 8 May 2017).

[5] Wahlstrom J, Karvosenoja N, Porvari P, Finnish Environment Institute, Helsinki (2006).

[6] Kruse N, Frennet A, Bastin JM, Catalysis Automotive Pollution Control IV, 116, 199 (1998)

[7] Despres J, Elsener M, Koebel M, Krocher O, Schnyder B, Wokaun A, Appl. Catal. B: Environ., 50(2), 73 (2004)

[8] Fernandes DM, Scofield CF, Neto AA, Cardoso MJB, Zotin FMZ, Chem. Eng. J., 160(1), 85 (2010)

[9] Ponce S, Pena MA, Fierro JLG, Appl. Catal. B: Environ., 24(3-4), 193 (2000)

[10] Wen Y, Zhang C, He H, Yu Y, Teraoka Y, Catal. Today, 126(3-4), 400 (2007)

[11] Kim CH, Qi GS, Dahlberg K, Li W, Science, 327(5973), 1624 (2010)

[12] Meiqing S, Zhen Z, Jiahao C, Yugeng S, Jun W, Xinquan W, J. Rare Earths, 31, 119 (2013)

[13] Yoon DY, Lim E, Kim YJ, Kim JH, Ryu T, Lee S, Cho BK, Nam IS, Choung JW, Yoo S, J. Catal., 319, 182 (2014)

[14] Wang J, Su Y, Wang X, Chen J, Zhao Z, Shen M, Catal. Commun., 25, 106 (2012)

[15] Zhou C, Liu X, Wu C, Wen Y, Xue Y, Chen R, Wang WG, Phys. Chem. Chem. Phys., 16, 5106 (2014)

[16] Najjar H, Lamonier JF, Mentre O, Giraudon JM, Batis H, Appl. Catal. B: Environ., 106(1-2), 149 (2011)

[17] Arai H, Yamada T, Eguchi K, Seiyama T, Appl. Catal., 26, 265 (1986)

[18] Bedel L, Roger AC, Estournes C, Kiennemann A, Catal. Today, 85(2-4), 207 (2003)

[19] Shannon RD, Acta Crystallogr. A, 32, 751 (1976)

[20] Lobos S, Ganne M, Bohan L, Simposio Iberoameriano de Catalisis, II, 1267 (1998).

[21] Hadjiivanov K, Catal. Lett., 68(3-4), 157 (2000)

[22] Tang N, Liu Y, Wang HQ, Wu ZB, J. Phys. Chem. C, 115, 8214 (2011)

[23] Sedlmair C, Seshan K, Jentys A, Lercher JA, J. Catal., 214(2), 308 (2003)

[24] Baltrusaitis J, Schuttlefield J, Jensen JH, Grassian VH, Phys. Chem. Chem. Phys., 9, 4971 (2007)

[25] Thampy S, Zheng YP, Dillon S, Liu CF, Jangjou Y, Lee YJ, Epling WS, Xiong K, Chabal YJ, Cho K, Hsu JWP, Catal. Today, 310, 195 (2018)

[26] Machida M, Uto M, Kurogi D, Kijima T, Chem. Mater., 12, 3158 (2000)

[27] Huang SJ, Walters AB, Vannice MA, J. Catal., 192(1), 29 (2000)

[28] Luo JY, Gao F, Kim DH, Peden CHF, Catal. Today, 231, 164 (2014)

[29] Merino NA, Barbero BP, Ruiz P, Cadus LE, J. Catal., 240(2), 245 (2006)

[30] de la Cruz RMG, Falcon H, Pena MA, Fierro JLG, Appl. Catal. B: Environ., 33(1), 45 (2001)

[31] Majewski WA, Ambs JL, Bickel K, SAE Technical Paper 950374 (1995).

[32] Schmitz PJ, Kudla RJ, Drews AR, Chen AE, Lowe-Ma CK, McCabe RW, Schneider WF, Goralski CT, Appl. Catal. B: Environ., 67(3-4), 246 (2006)