Cu-SSZ-13 catalyst for removing NOx with NH3 selective catalytic reduction technology
ZHAO Xiao-ge1, LIU Meng-meng2, WANG Jian-cheng2, HU Jiang-liang2, HAN Li-na1,2
1. College of Materials Science and Engineering, Taiyuan University of Technology, Taiyuan 030024, China; 2. Key Laboratory of Coal Science and Technology of the Ministry of Education and Shanxi Province, Taiyuan University of Technology, Taiyuan 030024, China
Abstract: Nitrogen oxides (NOx) in the exhaust gas from diesel vehicles are increasingly threatening human health and ecological environment.Due to its wide temperature window,excellent hydrothermal stability and other performances,Cu-SSZ-13 molecular sieve catalyst for removal of NOx is attracting more attentions.In order to meet the legislative emission requirements for NOx-containing exhaust gases and improve the NH3 selective catalytic reduction (NH3-SCR) reactive performances of Cu-SSZ-13 molecular sieve catalyst,it is necessary to study deeply the physicochemical properties of Cu-SSZ-13 catalyst and their influences on the reaction mechanism of NH3-SCR.This paper summarizes the recent research progress in Cu-SSZ-13 catalyst and its NH3-SCR reaction mechanism.This paper also describes in detail the changes of Cu active species of Cu-SSZ-13 catalyst in the reaction and compares the different preparation methods of Cu-SSZ-13 catalyst.The problems and suggestions in the study of Cu-SSZ-13 catalyst for removal of NOx with NH3-SCR technology are put forward.
赵小鸽, 刘梦梦, 王建成, 胡江亮, 韩丽娜. Cu-SSZ-13分子筛NH3-SCR脱硝技术研究[J]. 现代化工, 2017, 37(9): 34-39.
ZHAO Xiao-ge, LIU Meng-meng, WANG Jian-cheng, HU Jiang-liang, HAN Li-na. Cu-SSZ-13 catalyst for removing NOx with NH3 selective catalytic reduction technology. Modern Chemical Industry, 2017, 37(9): 34-39.
[1] Han S,Ye Q,Cheng S,et al.Effect of the hydrothermal aging temperature and Cu/Al ratio on the hydrothermal stability of CuSSZ-13 catalysts for NH3-SCR[J].Catalysis Science & Technology,2017,7:703-717. [2] Wang J,Zhao H,Haller G,et al.Recent advances in the selective catalytic reduction of NOx with NH3 on Cu-chabazite catalysts[J].Applied Catalysis B Environmental,2017,202:346-354. [3] Wang J,Peng Z,Qiao H,et al.Cerium-stabilized Cu-SSZ-13 catalyst for the catalytic removal of NOx by NH3[J].Industrial & Engineering Chemistry Research,2016,55(5):1-17. [4] Wang J,Peng Z,Ying C,et al.In-situ hydrothermal synthesis of Cu-SSZ-13/cordierite for the catalytic removal of NOx from diesel vehicles by NH3[J].Chemical Engineering Journal,2015,263(11):9-19. [5] Zhang T,Qiu F,Chang H,et al.Identification of active sites and reaction mechanism on low-temperature SCR activity over Cu-SSZ-13 catalysts prepared by different methods[J].Catalysis Science & Technology,2016,6:6294-6304. [6] Ren L,Zhu L,Yang C,et al.Designed copper-amine complex as an efficient template for one-pot synthesis of Cu-SSZ-13 zeolite with excellent activity for selective catalytic reduction of NOx by NH3[J].Chemical Communications,2011,47(35):9789-9791. [7] Martínez-Franco R,Moliner M,Thogersen J R,et al.Efficient one-pot preparation of Cu-SSZ-13 materials using cooperative OSDAs for their catalytic application in the SCR of NOx[J].Chemcatchem,2013,5(11):3316-3323. [8] Chen B,Xu R,Zhang R,et al.An economical way to synthesize SSZ-13 with abundant ion-exchanged Cu+ for an extraordinary performance in selective catalytic reduction (SCR) of NOx by ammonia[J].Environmental Science & Technology,2014,48(23):13909-13916. [9] 冯晴,裴仁彦,刘红光,等.干胶转化法合成整体式SSZ-13分子筛[J].化工学报,2017,68(3):1231-1238. [10] 王艳悦,李玉平,贾坤,等.SAPO-34分子筛晶种辅助合成SSZ-13分子筛[J].天然气化工:C1化学与化工,2016,41(4):5-9. [11] Deka U,Lezcanogonzalez I,Weckhuysen B M,et al.Local environment and nature of Cu active sites in zeolite-based catalysts for the selective catalytic reduction of NOx[J].Acs Catalysis,2013,3(3):413-427. [12] Lomachenko K A,Borfecchia E,Negri C,et al.The Cu-CHA deNOx catalyst in action:Temperature-dependent NH3 selective catalytic reduction monitored by operando XAS and XES[J].Journal of the American Chemical Society,2016,138(37):12025-12028. [13] Gao F,Walter E D,Kollar M,et al.Understanding ammonia selective catalytic reduction kinetics over Cu/SSZ-13 from motion of the Cu ions[J].Journal of Catalysis,2014,319:1-14. [14] Hun K J,Zhu H,Lee J H,et al.Two different cationic positions in Cu-SSZ-13?[J].Chemical Communications,2012,48(39):4758-4760. [15] Szanyi J,Kwak J H,Zhu H,et al.Characterization of Cu-SSZ-13 NH3-SCR catalysts:An in situ FTIR study[J].Physical Chemistry Chemical Physics,2013,15(7):2368-2380. [16] Kwak J H,Varga T,Peden C H F,et al.Following the movement of Cu ions in a SSZ-13 zeolite during dehydration,reduction and adsorption:A combined in situ TP-XRD,XANES/DRIFTS study[J].Journal of Catalysis,2014,314(20):83-93. [17] Kwak J H,Tran D,Szanyi J,et al.The effect of copper loading on the selective catalytic reduction of nitric oxide by ammonia over Cu-SSZ-13[J].Catalysis Letters,2012,142(3):295-301. [18] Ma L,Cheng Y,Cavataio G,et al.Characterization of commercial Cu-SSZ-13 and Cu-SAPO-34 catalysts with hydrothermal treatment for NH3-SCR of NOx in diesel exhaust[J].Chemical Engineering Journal,2013,225(3):323-330. [19] Wang D,Jangjou Y,Liu Y,et al.A comparison of hydrothermal aging effects on NH3-SCR of NOx over Cu-SSZ-13 and Cu-SAPO-34 catalysts[J].Applied Catalysis B Environmental,2015,165:438-445. [20] Su W,Li Z,Peng Y,et al.Correlation of the changes in the framework and active Cu sites for typical Cu/CHA zeolites (SSZ-13 and SAPO-34) during hydrothermal aging[J].Physical Chemistry Chemical Physics,2015,17(43):29142-29149. [21] Wang J,Peng Z,Qiao H,et al.Influence of aging on in situ hydrothermally synthesized Cu-SSZ-13 catalyst for NH3-SCR reaction[J].Rsc Advances,2014,4(80):42403-42411. [22] Zhang R,Li Y,Zhen T.Ammonia selective catalytic reduction of NO over Fe/Cu-SSZ-13[J].Rsc Advances,2014,4(94):52130-52139. [23] Gao F,Wang Y,Washton N M,et al.Effects of alkali and alkaline earth cocations on the activity and hydrothermal stability of Cu/SSZ-13 NH3-SCR Catalysts[J].Acs Catalysis,2015,5(11):6780-6791. [24] Zhu H,Kwak J H,Peden C H F,et al.In situ DRIFTS-MS studies on the oxidation of adsorbed NH3 by NOx over a Cu-SSZ-13 zeolite[J].Catalysis Today,2013,205(5):16-23. [25] Ma L,Cheng Y,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. [26] Lezcanogonzalez I,Deka U,Arstad B,et al.Determining the storage,availability and reactivity of NH3 within Cu-Chabazite-based ammonia selective catalytic reduction systems[J].Physical Chemistry Chemical Physics,2014,16(4):1639-1650. [27] Su W,Chang H,Peng Y,et al.Reaction pathway investigation on the selective catalytic reduction of NO with NH3 over Cu/SSZ-13 at low temperatures[J].Environmental Science & Technology,2015,49(1):467-473. [28] Crandell D W,Zhu H,Yang X,et al.The mechanism of selective catalytic reduction of NOx on Cu-SSZ-13-a computational study[J].Dalton Transactions,2016,46:369-377. [29] Paolucci C,Parekh A A,Khurana I,et al.Catalysis in a cage:Condition-dependent speciation and dynamics of exchanged Cu cations in SSZ-13 zeolites[J].Journal of the American Chemical Society,2016,138(18):6028-6048. [30] Feng G,Mei D,Wang Y,et al.Selective catalytic reduction over Cu/SSZ-13:Linking homo-and heterogeneous catalysis[J].Journal of the American Chemical Society,2017,139:4935-4942.
