Low-temperature Removal of NO by Spherical Activated Carbon Loaded with MnOx-CeO2 and Melamine

doi:10.15541/jim20160109

Abstract

Abstract:

A spherical activated carbon (SAC) loaded with MnO_x-CeO₂ and melamine was prepared as the catalyst for selective catalytic reduction (SCR) of NO at low temperature (120-180℃). Physical and chemical properties of the catalysts were characterized by scanning electron microscopy-energy dispersive spectrometer (SEM-EDS), X-ray diffraction (XRD), and N₂ adsorption-desorption technologies, respectively. The results show that about 99% NO_x conversion for 8.8 h at 180℃ is achieved over the catalyst with 10% melamine and 8% Mn loading (the mole ratio of Mn:Ce was fixed at 1:1) under the condition of 0.1% NO, 8% O₂ and a space velocity of 6000 h^-1. When the calcination temperature is higher than 400℃, the melamine-SCR activity is decreased obviously due to the crystallinity of the metal oxides increasing. When melamine loading is more than 15%, the specific surface area and pore volume of the catalysts decrease significantly, leading to a decline in the stationary-state NO_x conversion. However, the increase of metal oxides loading and reaction temperature is found to be beneficial to melamine-SCR reactivity, and the stationary-state NO_x conversion is always maintained at about 99% over a wide concentration range of NO and O₂.

Key words: spherical activated carbon, MnOx-CeO₂, melamine, NO, selective catalytic reduction

CLC Number:

TQ174

LI Jun, PAN Lei, WANG Ji-Tong, LONG Dong-Hui, QIAO Wen-Ming, LING Li-Cheng. Low-temperature Removal of NO by Spherical Activated Carbon Loaded with MnO_x-CeO₂ and Melamine[J]. Journal of Inorganic Materials, 2016, 31(11): 1205-1211.

Figures/Tables 12

Fig. 1 SEM images of (a, b) 400-8(Mn-Ce)/SAC, (c) Mn and (d) Ce mapping on 400-8(Mn-Ce)/SAC

Fig. 2 XRD patterns of 8(Mn-Ce)/SAC calcinated at different temperatures(a) 300℃; (b) 400℃; (c) 500℃; (d) 600℃

Fig. 3 Nitrogen adsorption-desorption isotherms of SAC and 400-8(Mn-Ce)/SAC with different melamine loadings

Table 1 Porosity parameters of SAC and 400-8(Mn-Ce)/SAC with different melamine loadings

Sample	S_BET/(m²·g^-1)	S_mic/(m²·g^-1)	V_t/(cm³·g^-1)	V_mic/(cm³·g^-1)
SAC	1411	1295	0.62	0.52
400-8(Mn-Ce)/SAC	710	648	0.32	0.26
400-8(Mn-Ce)/SAC-5	661	603	0.29	0.25
400-8(Mn-Ce)/SAC-10	578	528	0.26	0.22
400-8(Mn-Ce)/SAC-15	476	428	0.22	0.17
400-8(Mn-Ce)/SAC-20	392	355	0.18	0.14

Fig. 4 Reactivity of NO with melamine on 400-8(Mn-Ce)/ SAC-10Reaction conditions: 0.1% NO, 8% O2, balance N2, reaction temperature = 180℃, space velocity = 6000 h-1

Fig. 5 Effect of calcination temperature on NOx conversion over melamine-supported catalystsReaction conditions: 0.1% NO, 8% O2, balance N2, reaction temperature = 180℃, space velocity= 6000 h-1

Fig. 6 Effect of metal oxides loading on NOx conversion over melamine-supported catalystsReaction conditions: 0.1% NO, 8% O2, balance N2, reaction temperature = 180℃, space velocity = 6000 h-1

Fig. 7 Effect of melamine loading on NOx conversion over melamine-supported 400-8(Mn-Ce)/SACReaction conditions: 0.1% NO, 8% O2, balance N2, reaction temperature = 180℃, space velocity = 6000 h-1

Table 2 Mole ratio of reacted NO to melamine supported on 400-8(Mn-Ce)/SAC

Material balance	400-8(Mn-Ce)/SAC-5	400-8(Mn-Ce)/SAC-10	400-8(Mn-Ce)/SAC-15	400-8(Mn-Ce)/SAC-20
Amount of melamine on sample /×10^-4 mol	2.02	4.04	6.06	8.08
Breakthrough time(BTT) /h	4.20	8.80	13.80	18.50
Total amount of supplied net NO until BTT /×10^-4 mol	11.30	23.70	37.10	49.80
Ratio of reacted NO to supplied net NO /%	99.50	99.60	99.40	96.80
Amount of removed NO /× 10^-4 mol	11.20	23.60	36.90	48.20
Mole ratio of reacted NO to melamine on the catalyst	5.50	5.80	6.10	6.00

Fig. 8 Effect of reaction temperature on NOx conversion over 400-8(Mn-Ce)/SAC-10Reaction conditions: 0.1% NO, 8% O2, balance N2, space velocity = 6000 h-1

Fig. 9 Effect of (a) NO concentration and (b) O2 concentration on NOx conversion over 400-8(Mn-Ce)/SAC-10Reaction conditions: 0.01%~0.1% NO, 0~8% O2, balance N2, reaction temperature = 180℃, space velocity = 6000 h-1

Fig. 10 Effect of space velocity on NOx conversion over 400-8(Mn-Ce)/SAC-10Reaction conditions: 0.1% NO, 8% O2, balance N2, reaction temperature = 180℃

References 24

[1]	BOSCH H, JANSSEN F.Catalytic reduction of nitrogen oxides: A review on the fundamentals and technology. Catalysis Today, 1988, 2(4): 369-532.
[2]	YUAN CONG-HUI, LIU HUA-YAN, LU HAN-FENG, et al.Catalytic oxidation-reductive absorption process for NOx removal in humid waste gas.Chinese Journal of Environmental Engineering, 2008, 2(9): 1207-1212.
[3]	YAO YAO, ZHANG SHU-LE, ZHONG QIN, et al.Low temperature selective catalytic reduction of NO over manganese supported on TiO2 nanotubes. Journal of Fuel Chemistry and Technology, 2011, 39(9): 694-701.
[4]	AN ZHONG-YI, ZHUO YU-QUN, CHEN CHANG-HE.Influence of calcinations temperature on the catalytic activity of Mn/TiO2 for NO oxidation.Journal of Fuel Chemistry and Technology, 2014, 42(3): 370-376.
[5]	GUO JING, LI CAI-TING, LU PEI, et al.Research on SCR Denitrification of MnOx/Al2O3 modified by CeO2 and its mechanism at low temperature.Environmental Science, 2011, 32(8): 2240-2246.
[6]	LI LI, HUANG HUA-CUN, WEI TENG-YOU, et al.Influence of cerium additive on selective catalytic reduction of NOx with MnOx/ACFN catalyst. Chemical industry and Engineering progress, 2013, 32(11): 2655-2660.
[7]	WANG YAN-LI, LI XIAO-XIAO, ZHAN LIANG, et al.Effect of metal additives on the catalytic performance of MnOx-CeO2 supported on activated carbon honeycomb in NO removal at low temperature. Journal of Fuel Chemistry and Technology, 2014, 42(11): 1365-1371.
[8]	OZKAN U S, KUMTHEKAR M W, CAI Y P.Selective catalytic reduction of nitric oxide over vanadia/titania catalysts: temperature-programmed desorption and isotopically labeled oxygen-exchange studies.Industrial & Engineering Chemistry Research, 1994, 33(12): 2924-2929.
[9]	SHIRAHAMA N, MOCHIDA I, KORAI Y, et al.Reaction of NO2 in air at room temperature with urea supported on pitch based activated carbon fiber.Applied Catalysis B: Environmental, 2004, 52(3): 173-179.
[10]	SHIRAHAMA N, MOCHIDA I, KORAI Y, et al.Reaction of NO with urea supported on activated carbons. Applied Catalysis B: Environmental, 2005, 57(4): 237-245.
[11]	MIYAWAKI J, SHIMOHARA T, SHIRAHAMA N, et al.Removal of NOx from air through cooperation of the TiO2 photocatalyst and urea on activated carbon fiber at room temperature.Applied Catalysis B: Environmental, 2011, 110: 273-278.
[12]	WANG Z, WANG Y L, WANG D J, et al.Low-temperature selective catalytic reduction of NO with urea supported on pitch-based spherical activated carbon.Industrial & Engineering Chemistry Research, 2010, 49(14): 6317-6322.
[13]	WANG Z, WANG Y L, LONG D H, et al.Kinetics and mechanism study of low-temperature selective catalytic reduction of NO with urea supported on pitch-based spherical activated carbon.Industrial & Engineering Chemistry Research, 2011, 50(10): 6017-6027.
[14]	ZENG Z, LU P, LI C, et al.Selective catalytic reduction (SCR) of NO by urea loaded on activated carbon fiber (ACF) and CeO2/ACF at 30℃: The SCR mechanism.Environmental Technology, 2012, 33(11): 1331-1337.
[15]	LU P, ZENG Z, LI C T, et al.Room temperature removal of NO by activated carbon fibres loaded with urea and La2O3. Environmental Technology, 2012, 33(9): 1029-1036.
[16]	CHEN H Y, VOSKOBOINIKOV T, SACHTLER W M H. Reaction intermediates in the selective catalytic reduction of NOx over Fe/ZSM-5. Journal of Catalysis, 1999, 186(1): 91-99.
[17]	JOUBERT E, COURTOIS X, MARECOT P, et al.The chemistry of DeNOx reactions over Pt/Al2O3: the oxime route to N2 or N2O.Journal of Catalysis, 2006, 243(2): 252-262.
[18]	YANG JUN-BING, KANG FEI-YU.Activated carbon spheres and their applications.Materials Review, 2002, 16(5): 59-61.
[19]	MACHIDA M, KUROGI D, KIJIMA T, et al.MnOx-CeO2 binary oxides for catalytic NOx sorption at low temperatures. Selective reduction of sorbed NOx.Chemistry of Materials, 2000, 12(10): 3165-3170.
[20]	MACHIDA M, UTO M, KUROGI D, et al.Solid-gas interaction of nitrogen oxide adsorbed on MnOx-CeO2: a DRIFTS study. Journal of Materials Chemistry, 2001, 11: 900-904.
[21]	QI G, YANG R T.Characterization and FTIR studies of MnOx-CeO2 catalyst for low-temperature selective catalytic reduction of NO with NH3.The Journal of Physical Chemistry B, 2004, 108(40): 15738-15747.
[22]	QI G, YANG R T, CHANG R.MnOx-CeO2 mixed oxides prepared by co-precipitation for selective catalytic reduction of NO with NH3 at low temperatures. Applied Catalysis B: Environmental, 2004, 51(2): 93-106.
[23]	ETTIREDDY P R, ETTIREDDY N, SMIRNIOTIS P G, et al.Investigation of the selective catalytic reduction of nitric oxide with ammonia over Mn/TiO2 catalysts through transient isotopic labeling and in situ FT-IR studies.Journal of Catalysis, 2012, 292: 53-63.
[24]	XIE J L, FANG D, CHEN X L, et al.Performance and mechanism about MnOx species included in MnOx/TiO2 catalysts for SCR at low temperature.Catalysis Communications, 2012, 28: 77-81.

Low-temperature Removal of NO by Spherical Activated Carbon Loaded with MnO_x-CeO₂ and Melamine

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