Selective catalytic reduction of NO with NH3 over activated carbon impregnated with melamine at low temperature
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摘要: 通过将三聚氰胺(M)浸渍在活性炭(AC)上制备了渗氮活性炭(ACM),研究了浸渍时间、煅烧温度等因素对ACM含氮量以及低温NH3-SCR脱硝活性的影响。结果表明,三聚氰胺浸渍后可以提高活性炭的低温脱硝活性,在80 ℃下ACM-5-900的NO转化率达到51.67%,而AC只有21.92%。采用BET、元素分析及XPS等分别对渗氮活性炭ACM的结构、表面含氮量以及含氮官能团分布进行分析,表明含氮官能团的存在形式而不是含氮量影响渗氮活性炭的低温脱硝活性。同时NO+O2-TPD结果表明,渗氮改性后脱硝活性提高主要是由于表面含氮官能团提高了活性炭对NO的吸附和氧化。另外,SO2的存在会抑制渗氮活性炭的低温脱硝活性。Abstract: N-doped activated carbons (ACM) was obtained by impregnated activated carbon (AC) with melamine (M). The relationship between the impregnated time and calcination temperature on the nitrogen content and NH3-SCR activity was investigated. Results showed that SCR activity of ACM was higher than original AC. For ACM-5-900 was about 51.67% at 80 ℃ while AC was about 21.92%. Characterizations of BET, element analysis and XPS were employed to study the structural properties, nitrogen contents and distribution of nitrogen-containing groups of ACM. Results indicated that NO conversion of ACM was influenced by the form of nitrogen-containing functional groups rather than the nitrogen content. The NO+O2-TPD revealed that nitrogen-containing surface groups of ACM facilitated the adsorption and oxidation of NO, leading to the higher NO conversion. However, SO2 played an inhibit role on NO conversion of ACM.
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Key words:
- DeNOx /
- activated carbon /
- SCR /
- N-containing groups
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于艳科, 何炽, 陈进生, 孟小然. 电厂烟气脱硝催化剂V2O5-WO3/TiO2失活机理研究[J]. 燃料化学学报, 2012, 40(11): 1359-1365. (YU Yan-ke, HE Chi, CHEN Jin-sheng, MENG Xiao-ran. Deactivation mechanism of de-NOx catalyst (V2O5-WO3/TiO2) used in coal fired power plant[J]. Journal of Fuel Chemistry Technology, 2012, 40(11): 1359-1365.) YUN B K, KIM M Y. Modeling the selective catalytic reduction of NOx by ammonia over a Vanadia-based catalyst from heavy duty diesel exhaust gases[J]. Appl Therm Eng, 2013, 50(1): 152-158. 焦峰斌, 张亚平, 沈凯, 孙克勤, 徐海涛, 周长城. γ-Al2O3对SCR脱硝催化剂V2O5-WO3/TiO2的改性研究[J]. 燃料化学学报, 2012, 40(10): 1258-1263. (JIAO Feng-bin, ZHANG Ya-ping, SHEN Kai, SUN Ke-qin, XU Hai-tao, ZHOU Chang-cheng. γ-Al2O3 modification on V2O5-WO3/TiO2 catalyst for selective catalytic reduction (SCR) of NO[J]. Journal of Fuel Chemistry Technology, 2012, 40(10): 1258-1263.) HUANG M C, TENG H. Nitrogen-containing carbons from phenol-formaldehyde resins and their catalytic activity in NO reduction with NH3[J]. Carbon, 2003, 41(5): 951-957. 马建蓉, 刘振宇, 郭士杰. 同时脱除烟气中硫和硝的V2O5/AC催化剂研究[J]. 燃料化学学报, 2005, 33(1): 5-11. (MA Jian-rong, LIU Zhen-yu, GUO Shi-jie. Simultaneuos removal of SO2 and NO by V2O5/AC catalyst[J]. Journal of Fuel Chemistry Technology, 2005, 33(1): 5-11.) 于英民, 郭瑞莉, 李春虎. 半焦吸附剂烟气脱硫脱硝性能[J]. 燃料化学学报, 2011, 39(5): 385-389. (YU Ying-min, GUO Rui-li, LI Chun-hu. Flue gas desulfurization and denitrification performance of the semi-coke adsorbents[J]. Journal of Fuel Chemistry Technology, 2011, 39(5): 385-389.) RATHORE R S, SRIVASTAVA D K, AGARVAL A K, VERMA N. Development of surface functionalized activated carbon fiber for control of NO and particulate matter[J]. J Hazard Mater, 2010, 173(1/3): 211-222. BASHKOVA S, BANDOSZ T J. The effects of urea modification and heat treatment on the process of NO2 removal by wood-based activated carbon[J]. J Colloid Interface Sci, 2009, 333(1): 97-103. SERP P, FIGUETREDO J L. Carbon materials for catalysis[M]. Hoboken: John Wiley &Sons, Inc, 2009. SZYM'NSK G S, GRZYBEK T, PAPP H. Influence of nitrogen surface functionalities on the catalytic activity of activated carbon in low temperature SCR of NO with NH3[J]. Catal Today, 2004, 90(1/2): 51-59. SAMOJEDEN B, KLINIK J, GRZYBEK T, SUORUN W, GLASER R, PAPP H. DeNOx properties of activated carbons modified with N-compounds. Kraków: V Krakowska Konferencja Modych Uczonych, 2010. NOWICKI P, PIETRZAK R, WACHOWSKA H. X-ray photoelectron spectroscopy study of nitrogen-enriched active carbons obtained by ammoxidation and chemical activation of brown and bituminous coals[J]. Energy Fuels, 2010, 24(2): 1197-1206. RAYMUNDO E, CZAORAL D, LINARES A, FIND J, WILD U, SCHLOGL R. Structural characterization of N-containing activated carbon fibers prepared from a low softening point petroleum pitch and a melamine resin[J]. Carbon, 2002, 40(4): 597-608. PIETRZAK R. XPS study and physico-chemical properties of nitrogen-enriched microporous activated carbon from high volatile bituminous coal[J]. Fuel, 2009, 88(10): 1871-1877. BOUDOU J P, PARENT P, SUAREZ F, VILLAR S, MARTINEZ A, TASCON J M D. Nitrogen in aramid-based activated carbon fibers by TPD, XPS and XANES[J]. Carbon, 2006, 44(12): 2452-2462. PIETRZAK R, WACHOWSKA H, NOWICKI P. Preparation of nitrogen-enriched activated carbons from brown coal[J]. Energy Fuels, 2006, 20(3): 1275-1280. LAHAYE J, NANSE G, BAGREEV A, STRELKO V. Porous structure and surface chemistry of nitrogen containing carbons from polymers[J]. Carbon, 1999, 37(4): 585-590. GRZYBEK T, KLINIK J, SAMOJEDEN B, SUPRUN V, PAPP H. Nitrogen-promoted active carbons as DeNOx catalysts. 1. The influence of modification parameters on the structure and catalytic properties[J]. Catal Today, 2008, 137(2/4): 228-234. IZQUIERDO M T, RUBIO B, MAYORAL C, ANDRES J M. Modifications to the surface chemistry of low-rank coal-based carbon catalysts to improve flue gas nitric oxide removal[J]. Appl Catal B: Environ, 2001, 33(4): 315-324. SOUSA J P S, PEREIRA M F R, FIGUEIREDO J L. NO oxidation over nitrogen doped carbon xerogels[J]. Appl Catal B: Environ, 2012, 125(21): 398-408. SOUSA J P S, PEREIRA M F R, FIGUEIREDO J L. Catalytic oxidation of NO to NO2 on N-doped activated carbons[J]. Catal Today, 2011, 176(1): 383-387. SOUSA J P S, PEREIRA M F R, FIGUEIREDO J L. Modified activated carbon as catalyst for NO oxidation[J]. Fuel Process Technol, 2013, 106(2): 727-733. WAN X K, SHI H X, ZOU X Q, GE P. Effect of nitrogen doping on the reduction of nitric oxide with activated carbon in the presence of oxygen[J]. J Zhejiang Univ Sci A, 2008, 9(1): 113-117. STOHR B, BOEHM H P, SCHLOGL R. Enhancement of the catalytic activity of activated carbons in oxidation reactions by thermal treatment with ammonia or hydrogen cyanide and observation of a superoxide species as a possible intermediate[J]. Carbon, 1991, 29(6): 707–720. STRELKO V V, KUTS V S, THROWER P A. On the mechanism of possible influence of heteroatoms of nitrogen,boron and phosphorusin a carbon matrix on the catalytic activity of carbons in electron transfer reactions[J]. Carbon, 2000, 38(10): 1499-1524.
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