Reaction Mechanism of H2-Assisted C3H6-SCR over Ag-CexZr Catalyst as Investigated by In situ FTIR

doi:10.1007/s40242-020-0026-1

Abstract

Abstract: A series of silver-doped cerium zirconium oxide(Ag-Ce_xZr) samples was synthesized successfully for selective catalytic reduction of nitric oxide(NO) with hydrogen and propene(H₂/C₃H₆-SCR) under excess oxygen condition. The catalytic activity test proved that Ag-Ce_0.4Zr exhibited the best C₃H₆-SCR activity. Hydrogen(H₂) significantly enhanced NO conversion and widened the temperature window. Multi-technology characterizations were conducted to ascertain the properties of fabricated catalysts including X-ray diffraction(XRD), Fourier transform infrared spectrometry(FTIR), scanning electron microscopy(SEM) and H₂ temperature programmed reduction (H₂-TPR). In situ FTIR results demonstrated that various types of nitrates and chelating nitrite were generated on Ag-Ce_xZr after introduction of NO. Besides, adding H₂ could increase the concentration of bidentate nitrate and chelated bidentate nitrate dramatically, especially for Ag-Ce_0.4Zr catalyst. Transient reaction between pre-adsorbing NO and C₃H₆/C₃H₆+H₂ illuminated that the most active intermediate was chelating nitrite,which was promoted significantly by H₂ participation. Furthermore, adding H₂ improved the formation of organo-nitro(R-NO₂), which was the key intermediate in C₃H₆-SCR. The reaction mechanism over Ag-Ce_xZr catalysts was proposed at 200℃ as follows:nitric oxide(NO)+propene(C₃H₆)+hydrogen(H₂)+oxygen(O₂)→chelating nitrite(NO₂^-)+acrylate-type species(C_xH_yO_z)→organo-nitro(R-NO₂)→isocyanate(-NCO)+cyanide(-CN)→nitrogen(N₂).

Key words: NO, H₂/C₃H₆-SCR, In situ Fourier transform infrared(FTIR) spectrometry

DUAN Jun, ZHAO Ling, GAO Shengjun, ZHANG Yu. Reaction Mechanism of H₂-Assisted C₃H₆-SCR over Ag-Ce_xZr Catalyst as Investigated by In situ FTIR[J]. Chemical Research in Chinese Universities, 2020, 36(5): 885-893.

References 38

[1]	Yuan D. L., Li X. Y., Zhao Q. D., Zhao J. J., Tadé M., Liu S. M., Catal., 2014, 309, 268
[2]	Goula M. A., Charisiou N. D., Papageridis K. N., Delimitis A., Papista E., Pachatouridou E., J. Environ. Chem. Eng., 2016, 4, 1629
[3]	Chaieb T., Delannoy L., Casale S., Louis C., Thomas C., Chem. Commun.(Camb.), 2015, 51, 796
[4]	Burch R., Cat. Rev., 2011, 46, 271
[5]	Luo J., Gao F., Kim D. H., Peden C. H. F., Catal. Today, 2014, 231, 164
[6]	Azis M. M., Härelind H., Creaser D., Chem. Eng. J., 2015, 278, 394
[7]	Miyadera T., Appl. Catal. B, 1993, 2, 199
[8]	Shimizu K. I., Satsuma A., Phys. Chem. Chem. Phys., 2006, 8, 2677
[9]	Yamaguchi A., Goto I., Wang Z. M., Kumagai M., Stud. Surf. Sci. Catal., 1999, 121, 371
[10]	Sazama P., Capek L., Drobna H., Sobalik Z., Dedecek J., Arve K., J. Catal., 2005, 232, 302
[11]	Yu Y. B., He H., Zhang X. L., Deng H., Catal. Sci. Technol., 2014, 4, 1239
[12]	Breen J. P., Burch R., Top. Catal., 2006, 39, 53
[13]	Sazama P., Wichterlova B., Chem. Commun.(Camb.), 2005, 14, 4810
[14]	Azis M. M., Härelind H., Creaser D., Catal. Sci. Technol., 2015, 5, 296
[15]	Xu G. Y., Yu Y. B., He H., J. Phys. Chem. C, 2018, 122, 670
[16]	Kalamaras C. M., Olympiou G. G., Pârvulescu V. I., Cojocaru B., Efstathiou A. M., Appl. Catal. B, 2017, 206, 308
[17]	Väliheikki A., Petallidou K. C., Kalamaras C. M., Kolli T., Huuhtanen M., Maunula T., Appl. Catal. B, 2014, 156/157, 72
[18]	Finocchio E., Daturi M., Binet C., Lavalley J. C., Blanchard G., Catal. Today, 1999, 52, 53
[19]	Faqeeh A. J., Ali T. T., Basahel S. N., Narasimharao K., Mol. Catal., 2018, 456, 10
[20]	Zhao L. K., Li C. T., Li S. H., Wang Y., Zhang J. Y., Wang T., Zeng G. M., Appl. Catal. B, 2016, 198, 420
[21]	Xu G. Y., Ma J. Z., Wang L., Xie W., Liu J. J., Yu Y. B., He H., Appl. Catal. B, 2019, 244, 909
[22]	Pietrzyk P., Podolska K., Sojka Z., J. Phys. Chem. C, 2011, 11, 13008
[23]	Azambre B., Atribak I., Bueno-LóPez A., GarcíA-GarcíA A., J. Phys. Chem. C, 2010, 114, 13300
[24]	Jiang H. X., Wang Q. Y., Wang H. Q., Chen Y. F., Zhang M. H., ACS Appl. Mater. Interfaces, 2016, 8, 26817
[25]	Bentrup U., Richter M., Fricke R., Appl. Catal. B, 2005, 55, 213
[26]	Richter M., Appl. Catal. B, 2004, 51, 261
[27]	Richter M., Abramova A., Bentrup U., Fricke R., J. Appl. Spectrosc., 2004, 71(3), 400
[28]	Satsuma A., Shibata J., Wada A., Shinozaki Y., Hattori T., Stud. Surf. Sci. Catal., 2003, 145, 235
[29]	Kameoka S., Kita K., Tanaka S. I., Nobukawa T., Ito S. I., Tomishige K., Catal. Lett., 2002, 79, 63
[30]	Yu Y., Bian Z. F., Song F. J., Wang J., Zhong Q., Kawi S., Top. Catal., 2018, 61, 1514
[31]	Meunier F. C., Breen J. P., Zuzaniuk V., Olsson M., Ross J. R. H., J. Catal., 1999, 187, 493
[32]	Liu B., Li C. M., Zhang G. Q., Yao X. S., Chuang S. S. C., Li Z., ACS Catal., 2018, 8, 10446
[33]	Amiridis M. D., Zhang T. J., Farrauto R. J., Appl. Catal. B, 1996, 10, 203
[34]	Zhang Z. X., Chen M. X., Jiang Z., Shangguan W. F., J. Environ. Sci., 2010, 22, 1441
[35]	Halkides T. I., Kondarides D. I., Verykios X. E., Catal. Today, 2002, 73, 213
[36]	Fritz A., Pitchon V., Appl. Catal. B, 1997, 13, 1
[37]	Parvulescu V. I., Grange P., Delmon B., Catal. Today, 1998, 46, 233
[38]	Yuan M. H., Deng W. Y., Dong S. L., Li Q. C., Zhao B. T., Su Y. X., Chem. Eng. J., 2018, 353, 839

Reaction Mechanism of H₂-Assisted C₃H₆-SCR over Ag-Ce_xZr Catalyst as Investigated by In situ FTIR

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