Abstract
SSZ-13 zeolite was synthesized using four templates, and the synthesis conditions with choline chloride (CC) as template were optimized by dynamic stirring, fluoride-assisted and seed-assisted synthesis. Because the geometric dimensions of CC dimer (7.21 × 10.72 Å) and CHA cage (7.3 × 12 Å) matched closely, the crystallinity and specific surface area of sample synthesized using CC were higher than those of other samples (except for that of the sample synthesized using TMAdaOH). By adopting three improved methods, SSZ-13 samples with better crystallinity, higher specific surface area and more regular morphology could be synthesized in a shorter time (3–4 days). The sample prepared using fluoride-assisted method could achieve a similar crystallinity to the sample synthesized using TMAdaOH. The corresponding catalyst exhibited the best catalytic performance in the NH3-SCR reaction, with 100% NO conversion from 150 to 550 °C. This performance was attributed to fluoride ions promoting the formation of CC dimers through charge attraction of SiF62−. Furthermore, by synthesis optimization, the more developed pore structure, stronger NH3 adsorption capacity and lower CuO content of Cu-SSZ-13 were also important factors for the improved catalytic performance.
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Yu QQ, Wang H, Liu T et al (2012) High-efficiency removal of NOx using a combined adsorption-discharge plasma catalytic process. Environ Sci Technol 46:2337–2344
Zhao B, Wang SX, Liu H et al (2013) NOx emissions in China: historical trends and future perspectives. Atmos Chem Phys 13:9869–9897
Fan C, Chen Z, Pang L et al (2018) The influence of Si/Al ratio on the catalytic property and hydrothermal stability of Cu-SSZ-13 catalysts for NH3-SCR. Appl Catal A 550:256–265
Kobayashi M, Kuma R, Morita A (2006) Low temperature selective catalytic reduction of NO by NH3 over V2O5 supported on TiO2-SiO2-MoO3. Catal Lett 112:37–44
Shan YL, Shi XY, Du JP et al (2019) Cu-exchanged RTH-type zeolites for NH3-selective catalytic reduction of NOx: Cu distribution and hydrothermal stability. Catal Sci Technol 9:106–115
Zha KW, Kang L, Feng C et al (2018) Improved NOx reduction in the presence of alkali metals by using hollandite Mn-Ti oxide promoted Cu-SAPO-34 catalysts. Environ Sci Nano 5:1408–1419
Wang JH, Zhao HW, Haller G et al (2017) Recent advances in the selective catalytic reduction of NOx with NH3 on Cu-Chabazite catalysts. Appl Catal B 202:346–354
Fickel DW, D’Addio E, Lauterbach JA, Lobo RF (2011) The ammonia selective catalytic reduction activity of copper-exchanged small-pore zeolites. Appl Catal B 102:441–448
Gao F, Hun J, Janos S, Peden CHF (2013) Current understanding of Cu-exchanged chazbazite molecular sieves for use as commercial diesel engine DeNOx Catalysts. Top Catal 56:1441–1459
Mu YY, Zhang Y, Fan JY, Guo CL (2017) Effect of ultrasound pretreatment on the hydrothermal synthesis of SSZ-13 zeolite. Ultrason Sonochem 38:430–436
Beale AM, Gao F, Lezcano-gonzalez I et al (2015) Recent advances in automotive catalysis for NOx emission control by small-pore microporous materials. Chem Soc Rev 44:7371–7405
Deka U, Eilertsen EA, Emerich H et al (2012) Confirmation of isolated Cu2+ ions in SSZ-13 zeolite as active sites in NH3-selective catalytic reduction. J Phys Chem C 116:4809–4818
Korhonen ST, Fickel DW, Lobo RF et al (2011) Isolated Cu2+ ions: active sites for selective catalytic reduction of NO. Chem Commun 47:800–802
Kwak JH, Tonkyn RG, Kim DH et al (2010) Excellent activity and selectivity of Cu-SSZ-13 in the selective catalytic reduction of NOx with NH3. J Catal 275:187–190
Chen HY, Wei ZH, Kollar M et al (2015) A comparative study of N2O formation during the selective catalytic reduction of NOx with NH3 on zeolite supported Cu catalysts. J Catal 329:490–498
Gómez-García MA, Pitchon V et al (2005) Pollution by nitrogen oxides : an approach to NOx abatement by using sorbing catalytic materials. Environ Int 31:445–467
Zones SI (1990) Direct hydrothermal conversion of cubic P zeolite to organozeolite SSZ-13. J Chem Soc Faraday Trans 86:3467–3472
Eilertsen EA, Arstad B, Svelle S et al (2012) Single parameter synthesis of high silica CHA zeolites from fluoride media. Microporous Mesoporous Mater 153:94–99
Zhao ZC, Yu R, Zhao RR et al (2017) Cu-exchanged Al-rich SSZ-13 zeolite from organotemplate-free synthesis as NH3-SCR catalyst: effects of Na+ ions on the activity and hydrothermal stability. Appl Catal B 217:421–428
Ren LM, Zhang YB, Zeng SJ et al (2012) Design and synthesis of a catalytically active Cu-SSZ-13 zeolite from a copper-amine complex template. Chin J Catal 33:92–105
Ren LM, Zhu LF, Yang CG et al (2011) 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. Chem Commun 47:9789–9791
Xie LJ, Liu FD, Ren LM et al (2014) Excellent performance of one-pot synthesized Cu-SSZ-13 catalyst for the selective catalytic reduction of NOx with NH3. Environ Sci Technol 48:566–572
Xie LJ, Liu FD, Shi XY et al (2015) Effects of post-treatment method and Na co-cation on the hydrothermal stability of Cu-SSZ-13 catalyst for the selective catalytic reduction of NOx with NH3. Appl Catal B 179:206–212
Shibata S, Itakura M, Ide Y et al (2011) FAU-LEV interzeolite conversion in fluoride media. Microporous Mesoporous Mater 138:32–39
Shayib RM, George NC, Seshadri R et al (2011) Structure-directing roles and interactions of fluoride and organocations with siliceous zeolite frameworks. J Am Chem Soc 133:18728–18741
Wang JC, Liu ZQ, Feng G et al (2013) In situ synthesis of CuSAPO-34/cordierite and its selective catalytic reduction of nitrogen oxides in vehicle exhaust: the effect of HF. Fuel 109:101–109
Shan YL, Shi XY, Du JP et al (2019) SSZ-13 Synthesized by solvent-free method: a potential candidate for NH3-SCRcatalyst with high activity and hydrothermal stability. Ind Eng Chem Res 58:5397–5403
Nada MH, Larsen SC (2017) Insight into seed-assisted template free synthesis of ZSM-5 zeolites. Microporous Mesoporous Mater 239:444–452
Wang L, Shao Y, Zhang J, Anpo M (2006) Synthesis of MCM-48 mesoporous molecular sieve with thermal and hydrothermal stability with the aid of promoter anions. Microporous Mesoporobus Mater 95:17–25
Chen GR, Sun QM, Yu JH (2017) Nanoseed-assisted synthesis of nano-sized SAPO-34 zeolites using morpholine as the sole template with superior MTO performance. Chem Commun 53:13328–13331
Perez-Pariente J, Martens JA, Jacobs PA (1988) Factors affecting the synthesis efficiency of zeolite BETA from aluminosilicate gels containing alkali and tetraethylammonium ions. Zeolites 8:46–53
Caullet P, Delmotte L, Faust AC, Guth JL (1995) Synthesis of zeolite Beta from nonalkaline fluoride aqueous aluminosilicate gels. Zeolites 15:139–147
Wang YH, Chen JY, Lei XR et al (2018) Preparation of high silica microporous zeolite SSZ-13 using solid waste silica fume as silica source. Adv Powder Technol 29:1112–1118
Sun Y, Yang Q, Zhang Y et al (2019) Synthesis, characterization and catalytic application of ZnPO molecular sieve in wastewater system. J Clean Prod 213:1165–1171
Han LN, Zhao XG, Yu HF et al (2018) Preparation of SSZ-13 zeolites and their NH3-selective catalytic reduction activity. Microporous Mesoporous Mater 261:126–136
Kerr GT (1969) Preparation and properties of ultrastable hydrogen zeolite Y. J Phys Chem 2594:2780–2782
Hincapie BO, Garces LJ, Zhang Q et al (2004) Synthesis of mordenite nanocrystals. Microporous Mesoporous Mater 67:19–26
Tsokanis EA (1992) Further investigations of nucleation by initial breeding in the AI-free NH4-ZSM-5 system. Zeolites 12:369–373
Wu QM, Meng XJ, Gao XH, Xiao FS (2018) Solvent-free synthesis of zeolites : mechanism and utility. Acc Chem Res 51:1396–1403
Gao F, Walter ED, Karp EM et al (2013) Structure-activity relationships in NH3-SCR over Cu-SSZ-13 as probed by reaction kinetics and EPR studies. J Catal 300:20–29
Niu C, Shi XY, Liu FD et al (2016) High hydrothermal stability of Cu-SAPO-34 catalysts for the NH3-SCR of NOx. Chem Eng J 294:254–263
Han S, Ye Q, Cheng SY et al (2017) Effect of the hydrothermal aging temperature and Cu/Al ratio on the hydrothermal stability of CuSSZ-13 catalysts for NH3-SCR. Catal Sci Technol 7:703–717
Wang J, Yu T, Wang XQ et al (2012) The influence of silicon on the catalytic properties of Cu/SAPO-34 for NOx reduction by ammonia-SCR. Appl Catal B 127:137–147
Liu N, Zhang RD, Li YX, Chen BH (2014) Local electric field effect of TMI (Fe Co, Cu)-BEA on N2O direct dissociation. J Phys Chem C 118:10944–10956
Chen BH, Xu RN, Zhang RD, Liu N (2014) Economical way to synthesize SSZ-13 with abundant ion-exchanged Cu+ for an extraordinary performance in selective catalytic reduction (SCR) of NOx by ammonia. Environ Sci Technol 48:13909–13916
Wang JC, Peng ZL, Chen Y et al (2015) In-situ hydrothermal synthesis of Cu-SSZ-13/cordierite for the catalytic removal of NOx from diesel vehicles by NH3. Chem Eng J 263:9–19
Zhang RD, Teoh WY, Amal R et al (2010) Catalytic reduction of NO by CO over Cu/CexZr1-xO2 prepared by flame synthesis. J Catal 272:210–219
Wang D, Jangjou Y, Liu Y et al (2015) A comparison of hydrothermal aging effects on NH3-SCR of NOx over Cu-SSZ-13 and Cu-SAPO-34 catalysts. Appl Catal B 165:438–445
Zhu HY, Kwak JH, Peden CHF, Szanyi J (2013) In situ DRIFTS-MS studies on the oxidation of adsorbed NH3 by NOx over a Cu-SSZ-13 zeolite. Catal Today 205:16–23
Zhang T, Qiu F, Chang HZ et al (2016) Identification of active sites and reaction mechanism on low-temperature SCR activity over Cu-SSZ-13 catalysts prepared by different methods. Catal Sci Technol 6:6294–6304
Lomachenko KA, Borfecchia E, Negri C et al (2016) The Cu-CHA deNOx catalyst in action: temperature-dependent NH3-assisted selective catalytic reduction monitored by operando XAS and XES. J Am Chem Soc 138:12025–12028
Acknowledgements
This work was supported by the National Natural Science Foundation of China (Grant Nos. U1862102, 21976012) and Fundamental Research Funds for the Central Universities (Grant Nos. XK1802-1, JD1903).
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Wang, X., Zhang, R., Wang, H. et al. Strategy on Effective Synthesis of SSZ-13 Zeolite Aiming at Outstanding Performances for NH3-SCR Process. Catal Surv Asia 24, 143–155 (2020). https://doi.org/10.1007/s10563-020-09300-w
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DOI: https://doi.org/10.1007/s10563-020-09300-w