负载铈-铜茶梗基生物炭联合脱硝除汞的性能研究
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摘要
为了获得廉价易得的可以同时脱硝除汞的吸附催化剂,选取云南普洱茶废弃茶梗为碳源,采用等体积浸渍的方法制备了不同二氧化铈(CeO_2)-氧化铜(CuO)(CeO_2-CuO)浸渍配合比的茶梗基生物炭。并运用氮气(N_2)吸附脱附、扫描电子显微镜(SEM)、X射线衍射(XRD)对吸附催化剂进行了表征。在100~300℃范围内,固定床模拟烟气条件下研究了联合去除的效果。研究结果表明:CeO_2和CuO的浸渍量都为4%(wt,质量分数),制得的茶梗基生物炭,在300℃条件下,对一氧化氮(NO)的降解率达到82.3%,在100℃条件下,对单质汞(Hg0)的降解率高达93.0%。
Yunnan Pu'er tea stem was chosen as carbon source,in order to getting inexpensive adsorption catalyst for simultaneous removal of nitrogen oxides and elemental mercury.Tea stem biochars with different impregnating ratio of cerium dioxide-copper oxide(CeO_2-CuO)were prepared by incipient impregnation method.The adsorption catalyst was characterized using nitrogen(N_2)adsorption-desorption,scanning electron microscopy(SEM)and X-ray diffraction(XRD).The catalysts' performance of simultaneous removal was investigated in fixed-bed system with the condition of simulated flue gas in the temperature range of 100℃to 300℃.The results showed that when the impregnation ratio of CeO_2 and CuO was 4 wt%(mass percentage),respectively,the obtained tea stem biochar had a degradation rate of 82.3% for nitric oxide(NO)at 300℃,the degradation rate of elemental mercury(Hg~0)was as high as 93.0% at 100℃.
Yunnan Pu'er tea stem was chosen as carbon source,in order to getting inexpensive adsorption catalyst for simultaneous removal of nitrogen oxides and elemental mercury.Tea stem biochars with different impregnating ratio of cerium dioxide-copper oxide(CeO_2-CuO)were prepared by incipient impregnation method.The adsorption catalyst was characterized using nitrogen(N_2)adsorption-desorption,scanning electron microscopy(SEM)and X-ray diffraction(XRD).The catalysts' performance of simultaneous removal was investigated in fixed-bed system with the condition of simulated flue gas in the temperature range of 100℃to 300℃.The results showed that when the impregnation ratio of CeO_2 and CuO was 4 wt%(mass percentage),respectively,the obtained tea stem biochar had a degradation rate of 82.3% for nitric oxide(NO)at 300℃,the degradation rate of elemental mercury(Hg~0)was as high as 93.0% at 100℃.
引文
[1]Zeng Z,Lu P,Li C,et al.Selective catalytic reduction(SCR)of NO by urea loaded on activated carbon fibre(ACF)and CeO2/ACF at 30℃:the SCR mechanism[J].Environmental Technology,2012,33(11):1331-1337.
[2]王建英,马丽萍.燃煤烟气中新型吸附剂改性蛭石研究进展[J].电力科技与环保,2012,28(3):20-21.
[3]Streets D G,Zhang Q,Wu Y.Projections of global mercury emissions in 2050[J].Environmental Science&Technology,2009,43(8):2983-2988.
[4]中国环境科学研究院.火电厂大气污染物排放标准:GB13223—2011[M].北京:中国环境科学出版社,2012,4-6.
[5]王泉海.煤燃烧过程中汞排放及其控制的实验及机理研究[D].武汉:华中科技大学,2006.
[6]Lee T,Bai H.Low temperature selective catalytic reduction of NOx with NH3over Mn-based catalyst:a review[J].Environmental Science,2016,3(2):261-289.
[7]Liu C,Shi J W,Gao C,et al.Manganese oxide-based catalysts for low-temperature selective catalytic reduction of NOx with NH3:a review[J].Applied Catalysis A General,2016,522(14):54-69.
[8]Zhu C,Duan Y,Wu C Y,et al.Mercury removal and synergistic capture of SO2/NO by ammonium halides modified rice husk char[J].Fuel,2016,172(5):160-169.
[9]Singh S,Nahil M A,Sun X,et al.Novel application of cotton stalk as a waste derived catalyst in the low temperature SCRdeNOxprocess[J].Fuel,2013,105(5):585-594.
[10]Shen B,Li G,Wang F,et al.Elemental mercury removal by the modified bio-char from medicinal residues[J].Chemical Engineering Journal,2015,272(13):28-37.
[11]Jiang X,Lu P,Li C,et al.Experimental study on a room temperature urea-SCR of NO over activated carbon fibre-supported CeO2-CuO[J].Environmental Technology,2013,34(5):591-598.
[12]徐文青,赵俊,王海蕊,等.TiO2负载Mn-Co复合氧化物催化剂上NO催化氧化性能[J].物理化学学报,2013,29(2):385-390.
[13]陈建涛.燃煤烟气除汞脱硝干法联合脱除吸附-催化剂及过程研究[D].昆明:昆明理工大学,2014.
[14]Li G,Shen B,Li F,et al.Elemental mercury removal using biocharpyrolyzed from municipal solid waste[J].Fuel Processing Technology,2015,133(5):43-50.
[15]Yang W,Liu F,Xie L,et al.Effect of V2O5additive on the SO2resistance of a Fe2O3/AC catalyst for NH3-SCR of NOx at low temperatures[J].Industrial&Engineering Chemistry Research,2016,55(10):2677-2685.
[16]Lu P,Xing Y,Li C,et al.A reusable material with high performance for removing NO at room temperature:performance,mechanism and kinetics[J].Catalysis Science&Technology,2015,6(10):3520-3528.
[17]Zhang T,Qu R,Su W,et al.A novel Ce-Ta mixed oxide catalyst for the selective catalytic reduction of NOx with NH3[J].Applied Catalysis B Environmental,2015,176/177(20):338-346.
[18]黄伟,孙盛凯,李玉杰,等.硝酸改性处理对活性炭性能的影响[J].生物质化学工程,2006,40(6):17-21.
[19]Shen B,Chen J,Yue S,et al.A comparative study of modified cotton biochar and activated carbon based catalysts in low temperature SCR[J].Fuel,2015,156(9):47-53.
[20]Wu Z,Jin R,Wang H,et al.Effect of ceria doping on SO2resistance of Mn/TiO2for selective catalytic reduction of NO with NH3at low temperature[J].Catalysis Communications,2009,10(6):935-939.
[21]宋忠贤,宁平,李昊,等.不同Ce/Mn摩尔比对CeO2-MnOx催化剂低温NH3选择性催化还原NO的影响[J].分子催化,2015,29(5):422-430.
[22]Buciuman F C,Patcas F,Hahn T.A spillover approach to oxidation catalysis over copper and manganese mixed oxides[J].Chemical Engineering&Processing,1999,38(4/6):563-569.
[2]王建英,马丽萍.燃煤烟气中新型吸附剂改性蛭石研究进展[J].电力科技与环保,2012,28(3):20-21.
[3]Streets D G,Zhang Q,Wu Y.Projections of global mercury emissions in 2050[J].Environmental Science&Technology,2009,43(8):2983-2988.
[4]中国环境科学研究院.火电厂大气污染物排放标准:GB13223—2011[M].北京:中国环境科学出版社,2012,4-6.
[5]王泉海.煤燃烧过程中汞排放及其控制的实验及机理研究[D].武汉:华中科技大学,2006.
[6]Lee T,Bai H.Low temperature selective catalytic reduction of NOx with NH3over Mn-based catalyst:a review[J].Environmental Science,2016,3(2):261-289.
[7]Liu C,Shi J W,Gao C,et al.Manganese oxide-based catalysts for low-temperature selective catalytic reduction of NOx with NH3:a review[J].Applied Catalysis A General,2016,522(14):54-69.
[8]Zhu C,Duan Y,Wu C Y,et al.Mercury removal and synergistic capture of SO2/NO by ammonium halides modified rice husk char[J].Fuel,2016,172(5):160-169.
[9]Singh S,Nahil M A,Sun X,et al.Novel application of cotton stalk as a waste derived catalyst in the low temperature SCRdeNOxprocess[J].Fuel,2013,105(5):585-594.
[10]Shen B,Li G,Wang F,et al.Elemental mercury removal by the modified bio-char from medicinal residues[J].Chemical Engineering Journal,2015,272(13):28-37.
[11]Jiang X,Lu P,Li C,et al.Experimental study on a room temperature urea-SCR of NO over activated carbon fibre-supported CeO2-CuO[J].Environmental Technology,2013,34(5):591-598.
[12]徐文青,赵俊,王海蕊,等.TiO2负载Mn-Co复合氧化物催化剂上NO催化氧化性能[J].物理化学学报,2013,29(2):385-390.
[13]陈建涛.燃煤烟气除汞脱硝干法联合脱除吸附-催化剂及过程研究[D].昆明:昆明理工大学,2014.
[14]Li G,Shen B,Li F,et al.Elemental mercury removal using biocharpyrolyzed from municipal solid waste[J].Fuel Processing Technology,2015,133(5):43-50.
[15]Yang W,Liu F,Xie L,et al.Effect of V2O5additive on the SO2resistance of a Fe2O3/AC catalyst for NH3-SCR of NOx at low temperatures[J].Industrial&Engineering Chemistry Research,2016,55(10):2677-2685.
[16]Lu P,Xing Y,Li C,et al.A reusable material with high performance for removing NO at room temperature:performance,mechanism and kinetics[J].Catalysis Science&Technology,2015,6(10):3520-3528.
[17]Zhang T,Qu R,Su W,et al.A novel Ce-Ta mixed oxide catalyst for the selective catalytic reduction of NOx with NH3[J].Applied Catalysis B Environmental,2015,176/177(20):338-346.
[18]黄伟,孙盛凯,李玉杰,等.硝酸改性处理对活性炭性能的影响[J].生物质化学工程,2006,40(6):17-21.
[19]Shen B,Chen J,Yue S,et al.A comparative study of modified cotton biochar and activated carbon based catalysts in low temperature SCR[J].Fuel,2015,156(9):47-53.
[20]Wu Z,Jin R,Wang H,et al.Effect of ceria doping on SO2resistance of Mn/TiO2for selective catalytic reduction of NO with NH3at low temperature[J].Catalysis Communications,2009,10(6):935-939.
[21]宋忠贤,宁平,李昊,等.不同Ce/Mn摩尔比对CeO2-MnOx催化剂低温NH3选择性催化还原NO的影响[J].分子催化,2015,29(5):422-430.
[22]Buciuman F C,Patcas F,Hahn T.A spillover approach to oxidation catalysis over copper and manganese mixed oxides[J].Chemical Engineering&Processing,1999,38(4/6):563-569.