Abstract：A rice husk-derived activated carbon supported Mn-Ce catalyst (Mn-Ce/DAC) was prepared by an impregnation method and tested for the selective catalytic reduction of NOx with NH3. Such catalysts were characterized by N2 adsorption, X-ray powder diffraction (XRD), X-ray photoelectron spectroscopy (XPS) and temperature programmed desorption (TPR/TPD). The characterization results indicated that Mn-Ce/DAC catalyst exhibited the higher Ce3+/Ce4+ ratio, chemisorbed oxygen and Brønsted acid sites than commercial sawdust-derived activated carbon supported Mn-Ce catalyst (Mn-Ce/MAC). All of these factors played significant roles in the high SCR activity and SO2 resistance. In situ DRIFTS results demonstrated that sulfate formation was suppressed on the surface of the DAC support, which might be the most significant reason that Mn-Ce/DAC maintained a high SCR activity in the presence of SO2.
束韫, 张凡, 王洪昌, 石应杰, 朱金伟. 稻壳基活性炭催化剂的低温NH3-SCR抗硫性能[J]. 中国环境科学, 2019, 39(11): 4620-4627.
SHU Yun, ZHANG Fan, WANG Hong-chang, SHI Ying-jie, ZHU Jin-wei. Sulfur resistance of rice husk based activated carbon catalyst for the low-temperature selective catalytic reduction of NO by NH3. CHINA ENVIRONMENTAL SCIENCECE, 2019, 39(11): 4620-4627.
Busca G, Lietti L, Ramis G, et al. Chemical and mechanistic aspects of the selective catalytic reduction of NOx by ammonia over oxide catalysts:A review[J]. Applied Catalysis B:Environmental, 1998,18:1-36.
[2]
Kobayashi M, Miyoshi K. WO3-TiO2 monolithic catalysts for high temperature SCR of NO by NH3:Influence of preparation method on structural and physico-chemical properties, activity and durability[J]. Applied Catalysis B:Environmental, 2007,72:253-261.
[3]
Topsoe N Y, Topsoe H, Dumesic J A. Vanadia/Titania catalysts for selective catalytic reduction (SCR) of nitric-oxide by ammonia:I. Combined temperature-programmed in-situ FTIR and on-line mass-spectroscopy studies[J]. Journal of Catalysis, 1995,151:226-240.
[4]
Liu Z M, Zhang S X, Li J H, et al. Novel V2O5-CeO2/TiO2 catalyst with low vanadium loading for the selective catalytic reduction of NOx by NH3[J]. Applied Catalysis B:Environmental, 2014,158-159:11-19.
[5]
Tang X L, Hao J M, Xu W G, et al. Low temperature selective catalytic reduction of NOx with NH3 over amorphous MnOx catalysts prepared by three methods[J]. Catalysis Communications, 2007,8:329-334.
[6]
Lee K J, Kumar P A, Maqbool M S, et al. Ceria added Sb-V2O5/TiO2 catalysts for low temperature NH3-SCR:Physico-chemical properties and catalytic activity[J]. Applied Catalysis B:Environmental, 2013, 142:705-717.
[7]
胡强,熊志波,白鹏,等.铈钛掺杂促进铁氧化物低温SCR脱硝性能的机理[J]. 中国环境科学, 2016,36(8):2304-2310. Hu Q, Xiong Z B, Bai P, et al. Mechanism of niobium titanium doping promoting low temperature SCR denitrification performance of iron oxide[J]. China Environmental Science, 2016,36(8):2304-2310.
[8]
姚小江,马凯莉,邹伟欣,等.制备方法对MnOx-CeO2催化剂理化性质及低温NH3-SCR脱硝性能的影响(英文)[J]. 催化学报, 2017,38(1):146-159. Yao X J, Ma K L, Zou W X, et al. Effect of preparation methods on physicochemical properties of MnOx-CeO2 catalyst and denitrification performance of NH3-SCR at low temperature (In English)[J]. Chinese Journal of Catalysis, 2017,38(1):146-159.
[9]
Liu C, Chen L, Li J H, et al. Enhancement of activity and sulfur resistance of CeO2 supported on TiO2-SiO2 for the selective catalytic reduction of NO by NH3[J]. Environ. Sci. Technol., 2012,46(11):6182-6189.
[10]
Nakashima H, Omae K, Takebayashi T, et al. Less expensive and more environmentally friendly silica precursor[J]. Journal of Occupational Health, 1998,40:270-275.
[11]
Peng Y, Liu C, Zhang X, et al. The effect of SiO2 on a novel CeO2-WO3/TiO2 catalyst for the selective catalytic reduction of NO with NH3[J]. Applied Catalysis B:Environmental, 2013,140-141:276-282.
[12]
Lin K, Han L, He J, et al. Improved NOx reduction in the presence of SO2 by using Fe2O3 promoted halloysite-supported CeO2-WO3 catalysts[J]. Environmental Science & Technology, 2019,53:938-945.
[13]
Nuithitikul K, Srikhun S, Hirunpraditkoon S. Influences of pyrolysis condition and acid treatment on properties of durian peel-based activated carbon[J]. Bioresource Technology, 2010,101:426-429.
[14]
Cha J S, Choi J, Ko J H, et al. The low-temperature SCR of NO over rice straw and sewage sludge derived char[J]. Chemical Engineering Journal, 2010,156:321-327.
[15]
Liu J, Su Y, Li Q, et al. Preparation of wheat straw based superabsorbent resins and their applications as adsorbents for ammonium and phosphate removal[J]. Bioresource Technology, 2013, 143:32-39.
[16]
Xu W, Yu Y, Zhang C, He H. Selective catalytic reduction of NO by NH3 over a Ce/TiO2 catalyst[J]. Catalysis Communications, 2008,9:1453-1457.
[17]
Gao R, Zhang D, Liu X, et al. Enhanced catalytic performance of V2O5-WO3/Fe2O3/TiO2 microspheres for selective catalytic reduction of NO by NH3[J]. Catalysis Science Technology, 2013,3:191-199.
[18]
Yan Q, Nie Y, Yang R, et al. Highly dispersed CuyAlOx mixed oxides as superior low-temperature alkali metal and SO2 resistant NH3-SCR catalyst[J]. Applied Catalysis A:General, 2017,538:37-50.
[19]
Muñiz J, Marbán G, Fuertes A B. Low temperature selective catalytic reduction of NO over modified activated carbon fibres[J]. Applied Catalysis B:Environmental, 2000,27:27-36.
[20]
Pınar T, Sevil Y. Review on a novel biosilica source for production of advanced silica-based materials:Wheat husk[J]. Asia-Pacific Journal of Chemical Engineering, 2019,14:2262-2276.
[21]
Pena D A, Uphade B S, Smirniotis P G. TiO2-supported metal oxide catalysts for low-temperature selective catalytic reduction of NO with NH3:I. Evaluation and characterization of first row transition metals[J]. Journal of Catalysis, 2004,221:421-431.
[22]
Romeo M, Bak K, Fallah J E, et al. XPS Study of the reduction of cerium dioxide[J]. Surface and interface analysis, 1993,20:508-512.
[23]
Dupin J C, Gonbeau D, Vinatier P, et al. Systematic XPS studies of metal oxides, hydroxides and peroxides[J]. Physical Chemistry Chemical Physics, 2000,2:1319-1324.
[24]
Fang J, Bi X, Si D, et al. Spectroscopic studies of interfacial structures of CeO2-TiO2 mixed oxides[J]. Applied Surface Science, 2007,253:8952-8961.
[25]
Li P, Xin Y, Li Q, et al. Ce-Ti amorphous oxides for selective catalytic reduction of NO with NH3:Confirmation of Ce-O-Ti active sites[J]. Environmental Science & Technology, 2012,46:9600-9605.
[26]
Vishwanathan V, Ki-Won J, Jae-Woo K, et al. Vapour phase dehydration of crude methanol to dimethyl ether over Na-modified H-ZSM-5catalysts[J]. Applied Catalysis A:General, 2004,276:251-255.
[27]
Li J H, Zhu Y Q, Ke R, et al. Improvement of catalytic activity and sulfur-resistance of Ag/TiO2-Al2O3 for NO reduction with propene under lean burn conditions[J]. Applied Catalysis B:Environmental, 2008,80:202-213.
[28]
Chen Y X, Jiang Y, Li W Z, et al. Adsorption and interaction of H2S/SO2 on TiO2[J]. Catalysis Today, 1999,50:39-47.
[29]
Wu Z B, Jiang B Q, Liu Y, et al. DRIFT study of manganese/titania-based catalysts for low-temperature selective catalytic reduction of NO with NH3[J]. Environmental Science & Technology, 2007,41:5812-5817.
[30]
Ramis G, Li Y, Busca G, et al. Adsorption, activiation, and oxidation of ammonia over SCR catalysts[J]. Journal of Catalysis, 1995,157(2):523-535.
[31]
Jiang B Q, Wu Z B, Liu Y, et al. DRIFT Study of the SO2 effect on low-temperature SCR reaction over Fe-Mn/TiO2[J]. Journal of Physical Chemistry C, 2010,114:4961-4966.
[32]
Muhammad S M, Anil K P, Heon P H. Novel sulfation effect on low-temperature activity enhancement of CeO2-added Sb-V2O5/TiO2 catalyst for NH3-SCR[J]. Applied Catalysis B:Environmental, 2014,152-153:28-37.
[33]
Liam J, Qing Y, Wan L. Ceria modified FeMnOx-enhanced performance and sulphur resistance for low-temperature SCR of NOx[J]. Applied Catalysis B:Environmental, 2017,206:203-215.
