Cu/HZSM-5催化剂低温NH3-SCR脱硝性能研究

炼油技术与工程 ›› 2022, Vol. 52 ›› Issue (2): 55-59.

Cu/HZSM-5催化剂低温NH₃-SCR脱硝性能研究

张相俊

中国石油化工股份有限公司济南分公司，山东省济南市 250100

收稿日期:2021-09-26 出版日期:2022-02-16 发布日期:2022-02-16
作者简介:张相俊，助理工程师，硕士研究生，2017年毕业于北京石油化工学院化学工程专业,主要研究方向为催化剂及助剂研究、石油炼制化工工艺。联系电话：18953187876,E-mail:zhxj.jnlh@sinopec.com。

Study on low temperature NH₃-SCR denitration performance of Cu/HZSM-5 catalyst

Zhang Xiangjun

SINOPEC Jinan Company, Jinan, Shandong 250100

Received:2021-09-26 Online:2022-02-16 Published:2022-02-16

摘要/Abstract

摘要： 采用浸渍法制备Cu(x)/HZSM-5系列催化剂并应用于低温NH₃选择性催化还原脱硝性能研究。在固定床微型反应器上进行了O₂存在条件下催化剂的NH₃选择性催化还原NO活性评价，并通过XRD(X射线衍射仪)，SEM(扫描电子显微镜)，NO-TPD(程序升温脱附)，O₂-TPD，TG-DSC-MS(热重-差示扫描量热法-质谱联用)等对催化剂性能进行表征。结果表明，催化剂的催化脱硝活性随着Cu负载量增加而逐渐增强，Cu负载量影响催化剂表面活性物种分布、氧化还原性能和吸附脱附性能，Cu以CuO的形式存在于催化剂表面或空隙中。Cu(6)/HZSM-5表现出较好的低温脱硝性能，与其拥有较好的氧化性能和NO吸附脱附性能等有关，159~378 ℃时NO的转化率接近100%。

关键词: Cu/HZSM-5催化剂, 低温, NH₃-SCR, 脱硝, 吸附和脱附特性, 氧化性, 热重差热, 活性

Abstract: Cu(x)/HZSM-5 catalyst is prepared by impregnation method and applied to the denitration performance study of NH₃ selective catalytic reduction (NH₃-SCR) at low temperature. The NH₃-SCR denitration activity of the catalyst in the presence of O₂ is evaluated in a fixed bed microreactor, and the performance of the catalyst is characterized by XRD, SEM, NO-TPD, O₂-TPD and TG-DSC-MS. The denitration activity of the catalyst increases gradually with the increase of Cu loading. Cu loading affects the surface active species distribution, redox and adsorption desorption performance of the catalyst. Cu exists on the surface or voids of the catalyst in the form of CuO. Cu(6)/HZSM-5 shows good low-temperature denitration performance which is related to its good oxidation performance and NO adsorption and desorption performance. The conversion of NO is close to 100% at 159~378 ℃.

Key words: Cu/HZSM-5 catalyst, low temperature, NH₃-SCR, denitration, adsorption and desorption characteristics, oxidizability, thermogravimetric differential thermal, activity

张相俊. Cu/HZSM-5催化剂低温NH₃-SCR脱硝性能研究[J]. 炼油技术与工程, 2022, 52(2): 55-59.

Zhang Xiangjun. Study on low temperature NH₃-SCR denitration performance of Cu/HZSM-5 catalyst[J]. Petroleum Refinery Engineering, 2022, 52(2): 55-59.

参考文献

[1] ROY P O,HUIJBREGTS M,DESCHNES L,et al.Spatially-differentiated atmospheric source-receptor relationships for nitrogen oxides,sulfur oxides and ammonia emissions at the global scale for life cycle impact assessment[J].Atmospheric environment,2012,62:74-81.

[2] 徐涛,汪根宝,范艺.制氢转化炉低温SCR脱硝技术的应用[J].炼油技术与工程,2021,51 (9) :28-31.

[3] CHEN Z C,LI Z Q,ZHU Q Y,et al.Gas/particle flow and combustion characteristics and NOx emissions of a new swirl coal burner [J].Energy,2011,36(2):709-723.

[4] YANG S J,LI J H,WANG C Z,et al.Fe-Ti spinel for the selective catalytic reduction of NO with NH₃:mechanism and structure-activity relationship[J].Applied catalysis B:environmental,2012,117/118:73-80.

[5] KOC A B,ABDULLAH M.Performance and NOx emissions of a diesel engine fueled with biodiesel-diesel-water nanoemulsions [J].Fuel processing technology,2013,109:70-77.

[6] 朴佳锐,王骞,刘其武,等.催化法降低氮氧化物排放量的研究进展[J].石化技术与应用,2013,31(1):74-77.

[7] 杨宏军,朱礼想,李胜利,等.火电厂降低NOx排放的技术研究[J].电力科技与环保,2011,27(6):10-13.

[8] ZHAO P T,CHEN H F,GE S F,et al.Effect of the hydrothermal pretreatment for the reduction of NO emission from sewage sludge combustion [J].Applied energy,2013,111:199-205.

[9] LU B H,JIANG Y,CAI L L,et al.Enhanced biological removal of NOx from flue gas in a biofilter by Fe(Ⅱ)Cit/Fe(Ⅱ)EDTA absorption[J].Bioresource technology,2011,102(17):7707-7712.

[10] ZHANG X Y,JIN R F,LIU G F,et al.Removal of nitric oxide from simulated flue gas via denitrification in a hollow-fiber membrane bioreactor [J].Journal of environmental sciences,2013,25(11):2239-2246.

[11] KWON Y K,HAN D H.Microwave Effect in the Simultaneous Removal of NOx and SO₂ under electron beam irradiation and kinetic investigation of NOx removal rate [J].Industrial & engineering chemistry research,2010,49(17):8147-8156.

[12] FU S L,SONG Q,TANG J S,et al.Effect of CaO on the selective non-catalytic reduction deNOx process: experimental and kinetic study[J].Chemical engineering journal,2014,249:252-259.

[13] 马涛,王睿.NOx的催化分解研究[J].化学进展,2008, 20(6):798-810.

[14] 冯云桑,刘少光,陈成武,等.低温脱硝催化剂的研究现状[J].环境工程,2013,31(S1):373-377.

[15] 刘华南,何林,江书宇,等.低温选择性催化还原脱硝催化剂的研究现状与发展[J].四川环境,2013,32(3):117-122.

[16] ZHANG Q L,XU H D,QIU C T,et al.Catalytic performance and steady-state kinetics of Cu-ZSM-5 for selective catalytic reduction of NO with NH3[J].Acta physico-chimica sinica,2012,28(5):1230-1236.

[17] BRANDENBERGER S,KRCHER O,CASAPU M,et al.Hydrothermal deactivation of Fe-ZSM-5 catalysts for the selective catalytic reduction of NO with NH3[J].Applied catalysis B:environmental,2011,101(3/4):649-659.

[18] MA L,CHENG Y S,CAVATAIO G,et al.In situ DRIFTS and temperature-programmed technology study on NH₃-SCR of NOx over Cu-SSZ-13 and Cu-SAPO-34 catalysts [J].Applied catalysis B:environmental,2014,156/157:428-437.

[19] ZHANG T,LIU J,WANG D X,et al.Selective catalytic reduction of NO with NH₃ over HZSM-5-supported Fe-Cu nanocomposite catalysis:the Fe-Cu bimetallic effect [J].Applied catalysis B:environmental,2014,148/149:520-531.

[20] PANAHI P N,SALARI D,NIAEI A,et al.NO reduction over nanostructure M-Cu/ZSM-5 (M:Cr,Mn,Co and Fe) bimetallic catalysts and optimization of catalyst preparation by RSM [J].Journal of industrial and engineering chemistry,2013,19(6):1793-1799.

[21] WANG D,ZHANG L,LI J H,et al.NH₃-SCR over Cu/SAPO-34-Zeolite acidity and Cu structure changes as a function of Cu loading [J].Catalysis today,2014,231:64-74.

[22] SIERRA-PEREIRA C A,URQUIETA-GONZALEZ E A.Reduction of NO with CO on CuO or Fe₂O₃ catalysts supported on TiO₂ in the presence of O₂,SO₂ and water steam [J].Fuel,2014,118:137-147.

Cu/HZSM-5催化剂低温NH₃-SCR脱硝性能研究

Study on low temperature NH₃-SCR denitration performance of Cu/HZSM-5 catalyst

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