半干法高活性脱硝剂的制备及其脱硝性能
|
摘要
针对工业上100℃以下的中低温NO废气处理成本高、脱除困难等问题,以氢氧化钙为吸收剂、过碳酸钠为氧化剂,制备用于烟气半干法同时脱硫脱硝的高活性脱硝剂,并研究了NO去除率的影响因素。当气体总流量为1.2 L/min、O_2体积分数为10%、SO_2质量浓度1 428 mg/m~3、N_2为载气时,适宜的工艺条件为:氧化剂与吸收剂质量比5∶8、高活性脱硝剂中液固比80%、反应温度60℃、入口NO质量浓度670 mg/m~3。在此条件下,NO去除率达到55%以上,SO_2去除率达到100%。
In order to solve the high cost and difficulties in removing NO from medium and low temperature NO exhaust gas below 100℃ in the industry,a high-activity denitrfying agent was prepared by taking calcium hydroxide as absorbent and sodium percarbonate as oxidant for simultaneous desulfurization and denitrification of flue gas by semidry method. And the factors affecting the NO removal rate were studied. When the total gas flow rate is 1.2 L/min,O_2 volume fraction is 10%,SO_2 mass concentration is 1 428 mg/m~3,and N_2 is the carrier gas,suitable process conditions are as follows:mass ratio of oxidant to absorbent 5∶8,liquid-solid ratio of the high active denitrfying agent 80%,reaction temperature 60 ℃,and inlet NO concentration 670 mg/m~3. Under these conditions,the NO removal rate is above 55% and the SO_2 removal rate is 100%.
In order to solve the high cost and difficulties in removing NO from medium and low temperature NO exhaust gas below 100℃ in the industry,a high-activity denitrfying agent was prepared by taking calcium hydroxide as absorbent and sodium percarbonate as oxidant for simultaneous desulfurization and denitrification of flue gas by semidry method. And the factors affecting the NO removal rate were studied. When the total gas flow rate is 1.2 L/min,O_2 volume fraction is 10%,SO_2 mass concentration is 1 428 mg/m~3,and N_2 is the carrier gas,suitable process conditions are as follows:mass ratio of oxidant to absorbent 5∶8,liquid-solid ratio of the high active denitrfying agent 80%,reaction temperature 60 ℃,and inlet NO concentration 670 mg/m~3. Under these conditions,the NO removal rate is above 55% and the SO_2 removal rate is 100%.
引文
[1]钱定利，周飞翔，汪俊，等. silicalite-1全硅分子筛常温催化氧化NO性能[J].中国环境科学，2017,37(6):2080-2086.
[2] STREETS D G,WALDHOFF S T. Present and future emissions of air pollutants in China:SO2,NOx,and CO[J]. Atmos Environ,2000,34(3):363-374.
[3]乔南利，杨忆新，宋焕巧，等.低温NH3-SCR脱硝催化剂的研究现状与进展[J].化工环保，2017,37(3):282-288.
[4]卢朋，鲁卫哲，李欢，等.自蔓延高温燃烧合成法制备CeWTiOx催化剂及其NH3-SCR性能[J].燃料化学学报，2017,45(8):986-992.
[5] FORZATTI P. Present status and perspectives in de-NOx SCR catalysis[J]. Appl Catal A,2001,222(1/2):221-236.
[6] LONG R Q,YANG R T,CHANG R. Low temperature selective catalytic reduction(SCR)of NO with NH3 over Fe-Mn based catalyst[J]. Chem Commun,2002,5(5):452-453.
[7] SELLERI T,GRAMIGNI F,NOVA I,et al. NO oxidation on Fe-and Cu-zeolites mixed with BaO/Al2O3:free oxidation regime and relevance forthe NH3-SCR chemistry at low temperature[J]. Appl Catal B,2018,225:324-331.
[8] GUPTA H,BENSON S A,FAN L S,et al. Pilot-scale studies of NOx reduction by activated high-sodium lignite chars:a demonstration of the CARBONOX process[J].Ind Eng Chem Res,2004,43(18):5820-5827.
[9] SHAHRIAR K,ALI M K. Clean power production by simultaneous reduction of NOx and SOx contaminants using mazut nano-emulsion and wetflue gas desulfurization[J]. J Clean Prod,2018,201:229-235.
[10]凌绍华，景长勇，马婧，等.选择性非催化还原法烟气脱硝工业试验[J].化工环保，2013,33(4):304-307.
[11] BLUMRICH S,ENGLER B. The DESONOX/REDOX-process forflue gas cleaning:aflue gas purification process for the simultaneous removal of NOx and SO2 resp. CO and UHC[J]. Catal Today,1993,17(1/2):301-310.
[12] M?STBERG M,DAM-JOHANSEN K,JOHNSSON J E. Influence of mixing on the SNCR process[J].Chem Eng Sci,1997,52(15):2511-2525.
[13]刘华彦. NO的常温催化氧化及碱液吸收脱除NOx过程研究[D].杭州：浙江大学，2011.
[14]朱兆友，徐超，高秀，等. H2O2氧化-碱液吸收脱除NOx的工艺研究[J].化学与生物工程，2011,28:76-78.
[15] BHANARKAR A D,GUPTA R K,BINIWALE R B,et al. Nitric oxide absorption by hydrogen peroxide in airlift reactor:a study using response surface methodology[J]. Int J Environ Sci Technol,2014,11(6):1537-1548.
[16]周飞翔，汪俊，卢晗锋.金属阳离子对高硅分子筛催化氧化NO的影响[J].中国环境科学，2018,38(4):1287-1294.
[17]王飞，李兴强.烟气循环流化床同时脱硫脱硝技术研究[J].资源节约与环保，2015(9):18.
[18]许勇毅，查智明，赵翠仙.烟气循环流化床脱硫脱硝工艺技术的特点与现状[J].工业安全与环保，2007(1):16-17.
[19] ZHAO Y,GUO T X,ZANG Z L. Activity and characteristics of “oxygen-enriched” highly reactive absorbent for simultaneousflue gas desulfurization and denitrification[J]. Front Environ Sci Eng,2015,9(2):222-229
[20]李海宗.烟气循环流化床同时脱硫脱硝技术研究[D].保定：华北电力大学（河北），2005.
[121]周月桂，彭军，朱贤，等.过氧化氢溶液增湿Ca(OH)2脱硫的实验研究及微观机理分析[J].工程热物理学报，2009,30(3):513-516.
[22]朱贤，周月桂，柳瑶斌，等.过氧化氢水溶液增湿Ca(OH)2脱硫的实验研究[J].锅炉技术，2010,41(6):75-78.
[23]韩颖慧，赵毅，曹春梅，等.高分子过氧酸改性钙基添加剂烟气同时脱硫脱硝实验研究[J].中国电机工程学报，2012,32(35):31-36.
[24] ZHAO H K,TANG C,ZHANG D S,et al. Solidliquid equilibrium for the quaternary system of sodium carbonate+sodium chloride+hydrogen peroxide+water at 293.15 K[J]. J Chem Eng Data,2006,51(2):676-679.
[25]王香爱，陈养民.过碳酸钠的合成与应用[J].纯碱工业，2006(4):7-9.
[2] STREETS D G,WALDHOFF S T. Present and future emissions of air pollutants in China:SO2,NOx,and CO[J]. Atmos Environ,2000,34(3):363-374.
[3]乔南利，杨忆新，宋焕巧，等.低温NH3-SCR脱硝催化剂的研究现状与进展[J].化工环保，2017,37(3):282-288.
[4]卢朋，鲁卫哲，李欢，等.自蔓延高温燃烧合成法制备CeWTiOx催化剂及其NH3-SCR性能[J].燃料化学学报，2017,45(8):986-992.
[5] FORZATTI P. Present status and perspectives in de-NOx SCR catalysis[J]. Appl Catal A,2001,222(1/2):221-236.
[6] LONG R Q,YANG R T,CHANG R. Low temperature selective catalytic reduction(SCR)of NO with NH3 over Fe-Mn based catalyst[J]. Chem Commun,2002,5(5):452-453.
[7] SELLERI T,GRAMIGNI F,NOVA I,et al. NO oxidation on Fe-and Cu-zeolites mixed with BaO/Al2O3:free oxidation regime and relevance forthe NH3-SCR chemistry at low temperature[J]. Appl Catal B,2018,225:324-331.
[8] GUPTA H,BENSON S A,FAN L S,et al. Pilot-scale studies of NOx reduction by activated high-sodium lignite chars:a demonstration of the CARBONOX process[J].Ind Eng Chem Res,2004,43(18):5820-5827.
[9] SHAHRIAR K,ALI M K. Clean power production by simultaneous reduction of NOx and SOx contaminants using mazut nano-emulsion and wetflue gas desulfurization[J]. J Clean Prod,2018,201:229-235.
[10]凌绍华，景长勇，马婧，等.选择性非催化还原法烟气脱硝工业试验[J].化工环保，2013,33(4):304-307.
[11] BLUMRICH S,ENGLER B. The DESONOX/REDOX-process forflue gas cleaning:aflue gas purification process for the simultaneous removal of NOx and SO2 resp. CO and UHC[J]. Catal Today,1993,17(1/2):301-310.
[12] M?STBERG M,DAM-JOHANSEN K,JOHNSSON J E. Influence of mixing on the SNCR process[J].Chem Eng Sci,1997,52(15):2511-2525.
[13]刘华彦. NO的常温催化氧化及碱液吸收脱除NOx过程研究[D].杭州：浙江大学，2011.
[14]朱兆友，徐超，高秀，等. H2O2氧化-碱液吸收脱除NOx的工艺研究[J].化学与生物工程，2011,28:76-78.
[15] BHANARKAR A D,GUPTA R K,BINIWALE R B,et al. Nitric oxide absorption by hydrogen peroxide in airlift reactor:a study using response surface methodology[J]. Int J Environ Sci Technol,2014,11(6):1537-1548.
[16]周飞翔，汪俊，卢晗锋.金属阳离子对高硅分子筛催化氧化NO的影响[J].中国环境科学，2018,38(4):1287-1294.
[17]王飞，李兴强.烟气循环流化床同时脱硫脱硝技术研究[J].资源节约与环保，2015(9):18.
[18]许勇毅，查智明，赵翠仙.烟气循环流化床脱硫脱硝工艺技术的特点与现状[J].工业安全与环保，2007(1):16-17.
[19] ZHAO Y,GUO T X,ZANG Z L. Activity and characteristics of “oxygen-enriched” highly reactive absorbent for simultaneousflue gas desulfurization and denitrification[J]. Front Environ Sci Eng,2015,9(2):222-229
[20]李海宗.烟气循环流化床同时脱硫脱硝技术研究[D].保定：华北电力大学（河北），2005.
[121]周月桂，彭军，朱贤，等.过氧化氢溶液增湿Ca(OH)2脱硫的实验研究及微观机理分析[J].工程热物理学报，2009,30(3):513-516.
[22]朱贤，周月桂，柳瑶斌，等.过氧化氢水溶液增湿Ca(OH)2脱硫的实验研究[J].锅炉技术，2010,41(6):75-78.
[23]韩颖慧，赵毅，曹春梅，等.高分子过氧酸改性钙基添加剂烟气同时脱硫脱硝实验研究[J].中国电机工程学报，2012,32(35):31-36.
[24] ZHAO H K,TANG C,ZHANG D S,et al. Solidliquid equilibrium for the quaternary system of sodium carbonate+sodium chloride+hydrogen peroxide+water at 293.15 K[J]. J Chem Eng Data,2006,51(2):676-679.
[25]王香爱，陈养民.过碳酸钠的合成与应用[J].纯碱工业，2006(4):7-9.
© 2004-2018 中国地质图书馆版权所有 京ICP备05064691号 京公网安备11010802017129号 地址：北京市海淀区学院路29号 邮编：100083 电话：办公室：(+86 10)66554848；文献借阅、咨询服务、科技查新：66554700 |