Deactivation of Honeycomb SCR Catalysts in High-Arsenic Coal-Fired Power Plant

doi:10.11930/j.issn.1004-9649.201903095

Abstract

Abstract: In this paper, the arsenic deactivation of honeycomb Selective Catalytic Reaction (SCR) catalysts in Huolinhe coal-fired power plant were studied. The denitrification activity of catalyst were tested and assessed at different time points of its life cycle. In addition, by utilizing X-ray fluorescence spectrometer, N₂ adsorption-desorption, mercury porosimetry and automatic chemisorption analyzer (NH₃-TPD and H₂-TPR), the chemical compositions and physicochemical properties of the catalysts were explored and analyzed. As it is shown from the results, the deposition of arsenic in the surface and micro pores of the catalysts led to the decrease of specific surface area and acidity of the catalyst, which was the major reason for the poisoning of the catalyst. Bench-scale catalyst test results show that the activity of catalysts dropped down to 69% of the new catalysts after only about 1 000 hours service, suggesting a very fast deactivation process compared to normal catalyst. To extend the catalyst lifetime, certain procedures for catalyst lifetime managements were proposed to slow down the arsenic poisoning process in the coal-fired power plant fueled with high-arsenic coal.

Key words: coal fired power plant, Huolinhe coal, high-arsenic coal, selective catalyst reduction, denitrification activity, arsenic posion, catalyst lifetime management

YAO Yan, MA Yunlong, YANG Xiaoning, ZHANG Huadong, WANG Lipeng. Deactivation of Honeycomb SCR Catalysts in High-Arsenic Coal-Fired Power Plant[J]. Electric Power, 2020, 53(6): 191-196.

Add to citation manager EndNote|Ris|BibTeX

URL: https://www.electricpower.com.cn/EN/10.11930/j.issn.1004-9649.201903095

https://www.electricpower.com.cn/EN/Y2020/V53/I6/191

References

[1] 李德波, 廖永进, 陆继东, 等. 燃煤电站SCR催化剂更换周期及策略优化数学模型[J]. 中国电力, 2013, 46(12): 118-121
LI Debo, LIAO Yongjin, LU Jidong, et al. Study on mathematical models for optimization of SCR catalyst replacement cycle and strategy[J]. Electric Power, 2013, 46(12): 118-121
[2] MUZIO L, SMITH R, MUNCY J, et al. Protocol for laboratory testing SCR catalyst samples[R]. Palo Alto, California, 2006.
[3] Guideline for the testing of DeNO_x catalysts: VGB-R 302 H-2010 [S]. 2010.
[4] 宋玉宝, 杨杰, 金理鹏, 等. SCR脱硝催化剂宏观性能评估和寿命预测方法研究[J]. 中国电力, 2016, 49(4): 17-22
SONG Yubao, YANG Jie, JIN Lipeng, et al. Study on methodology of SCR catalyst macroscopical performance evaluation and lifetime prediction[J]. Electric Power, 2016, 49(4): 17-22
[5] JENSEN O R, SLABIAK T, WHITE N. Arsenic resistant SCR catalysts[R]. Lyngby: Haldor Topsoe Inco, 2005.
[6] 孙克勤, 钟秦, 于爱华. SCR催化剂的砷中毒研究[J]. 中国环保产业, 2008(1): 40-42
SUN Keqin, ZHONG Qin, YU Aihua. Study on arsenic poisoning of SCR catalyst[J]. China Environmental Protection Industry, 2008(1): 40-42
[7] 高燕, 白向飞, 王越. 霍林河14^#煤中微量元素的分布赋存特征研究[J]. 煤炭转化, 2015, 38(2): 1-5
GAO Yan, BAI Xiangfei, WANG Yue. Distribution and occurrence of trace elements in 14^# Huolinhe coal[J]. Coal Conversion, 2015, 38(2): 1-5
[8] 王起超, 邵庆春, 康淑莲, 等. 煤中15种微量元素在燃烧产物中的分配[J]. 燃料化学学报, 1996, 24(2): 137-142
WANG Qichao, SHAO Qingchun, KANG Shulian, et al. Distribution of 15 trace elements in the combustion products of coal[J]. Journal of Fuel Chemistry and Technology, 1996, 24(2): 137-142
[9] HUMS E. Mechanistic effects of arsenic oxide on the catalytic components of DeNO_x catalysts[J]. Industrial & Engineering Chemistry Research, 1992, 31(4): 1030-1035.
[10] 沈伯雄, 熊丽仙, 刘亭. 负载型V₂O₅-WO₃/TiO₂催化剂的砷中毒研究[J]. 燃料化学学报, 2011, 39(11): 856-859
SHEN Boxiong, XIONG Lixian, LIU Ting. Study on arsenic poisoning for loading catalyst of V₂O₅-WO₃/TiO₂[J]. Journal of Fuel Chemistry and Technology, 2011, 39(11): 856-859
[11] 付建, 刘国, 薛志钢, 等. 燃煤电厂砷的动态分布及排放特征[J]. 中国电力, 2013, 46(3): 95-99
FU Jian, LIU Guo, XUE Zhigang, et al. Configuration distribution and emission characteristics of arsenic from coal-fired power plants[J]. Electric Power, 2013, 46(3): 95-99
[12] JAMES E, TONY E, WILLIAM H, et al. The impact of arsenic on coal fired power plants equipped with SCR [C]// ICAC 2002 forum, Operating Experience for Reducing NO_x Emissions. Houston, 2002.
[13] HANS J H, TOPSØE N Y, 崔建华. 选择催化还原(SCR)脱硝技术在中国燃煤锅炉上的应用(上)[J]. 热力发电, 2007, 36(8): 13-18
HANS J H, TOPSØE N Y, CUI Jianhua. Application of SCR denitrification technology onto coal-fired boilers in China[J]. Thermal Power Generation, 2007, 36(8): 13-18
[14] 王泉海, 刘迎晖, 张军营, 等. CaO对烟气中砷的形态和分布的影响[J]. 环境科学学报, 2003, 23(4): 549-551
WANG Quanhai, LIU Yinghui, ZHANG Junying, et al. Effect of CaO on the speciation of arsenic in flue gases[J]. Acta Scientiae Circumstantiae, 2003, 23(4): 549-551
[15] 张军营, 任德贻, 钟秦, 等. CaO对煤中砷挥发性的抑制作用[J]. 燃料化学学报, 2000, 28(3): 198-200
ZHANG Junying, REN Deyi, ZHONG Qin, et al. Restraining of arsenic volatility using lime in coal combustion[J]. Journal of Fuel Chemistry and Technology, 2000, 28(3): 198-200
[16] HUMS E. A catalytically highly-active, arsenic oxide resistant V-Mo-O phase-results of studying intermediates of the deactivation process of V₂O₅-MoO₃-TiO₂(anatase) DeNO_x catalysts[J]. Research on Chemical Intermediates, 1993, 19(5): 419-441.
[17] 姚燕, 王乐乐, 李乐田, 等. 燃煤电厂选择性催化还原脱硝催化剂砷中毒分析[J]. 热力发电, 2018, 47(10): 31-36
YAO Yan, WANG Lele, LI Letian, et al. Arsenic deactivation of honeycomb SCR catalysts in coal-fired power plants[J]. Thermal Power Generation, 2018, 47(10): 31-36
[18] GUO X Y. Poisoning and sulfation on vanadia SCR catalyst[D]. Utah: Brigham Young University, 2006.
[19] LANGE F C, SCHMELZ H, KNÖZINGER H. Infrared-spectroscopic investigations of selective catalytic reduction catalysts poisoned with arsenic oxide[J]. Applied Catalysis B: Environmental, 1996, 8(2): 245-265.
[20] SHEN Boxiong, YAO Yan, CHEN Jianhong, et al. Alkali metal deactivation of Mn-CeO_x/Zr-delaminated-clay for the low-temperature selective catalytic reduction of NO_x with NH₃[J]. Microporous and Mesoporous Materials, 2013, 180: 262-269.
[21] TOPSOE N Y. Mechanism of the selective catalytic reduction of nitric oxide by ammonia elucidated by in situ on-line Fourier transform infrared spectroscopy[J]. Science, 1994, 265(5176): 1217-1219.