Acid-Alkaline Treatment of Mordenite and Its Catalytic Activity in the Hydrotreatment of Bio-Oil

https://doi.org/10.22146/ijc.51496

Febi Yusniyanti(1), Wega Trisunaryanti(2), Triyono Triyono(3*)

(1) Department of Chemistry, Islamic State University Maulana Malik Ibrahim, Jl. Gajayana No. 50, Dinoyo, Lowokawaru, Malang, 65144, Indonesia
(2) Department of Chemistry, Faculty of Mathematics and Natural Sciences, Universitas Gadjah Mada, Sekip Utara, Yogyakarta 55281, Indonesia
(3) Department of Chemistry, Faculty of Mathematics and Natural Sciences, Universitas Gadjah Mada, Sekip Utara, Yogyakarta 55281, Indonesia
(*) Corresponding Author

Abstract


Acid-alkaline treatment using acetic acid and sodium hydroxide (NaOH) were applied on mordenite (MOR) to increase the Si/Al ratio and surface area properties. Various time treatment (3, 6, and 9 h) and concentration of acetic acid (6, 9, and 12 M) were used to treat MOR, and followed by the treatment with NaOH (0.1 M) under room temperature. The MOR and treated mordenite were applied as a catalyst for hydrotreatment of cellulose-derived bio-oil. The acetic acid treatment caused the increase of the Si/Al ratio of mordenite up to 27.03. The Si/Al ratio was determined using ICP-AES analysis which was also confirmed using FT-IR analysis. The acidity was determined using NH3 vapors adsorption. The acidity test revealed that as the Si/Al ratio increased the acidity of mordenite decreased. The advantage of using acetic acid for acid treatment was that the XRD patterns of mordenite can be preserved with a little decrease of the intensity. On the other hand, the NaOH treatment under room temperature decreased the crystallinity down to 68%, which was calculated using XRD. The acid-alkaline treatment of mordenite succeeded to increase the surface area 2 times larger than the parent mordenite. The surface area was obtained from BET analysis. The acid-alkaline treated mordenite exhibited better catalytic activity upon hydrotreatment of biomass-derived bio-oil compared to the parent mordenite which corresponded to its highest surface area.


Keywords


acetic acid; bio-oil; dealumination; hydrotreatment; mordenite

Full Text:

Full Text PDF


References

[1] Paixão, V., Carvalho, A.P., Rocha, J., Fernandes, A., and Martins, A., 2010, Modification of MOR by desilication treatments: Structural, textural and acidic characterization, Microporous Mesoporous Mater., 131 (1-3), 350–357.

[2] Huang, S., Liu, X., Yu, L., Miao, S., Liu, Z., Zhang, S., and Xie, S., 2014, Preparation of hierarchical mordenite zeolites by sequential steaming-acid leaching-alkaline treatment, Microporous Mesoporous Mater., 191, 18–26.

[3] Groen, J.C., Sano, T., Moulijn, J.A., and Pérez-Ramírez, J., 2007, Alkaline-mediated mesoporous mordenite zeolites for acid-catalyzed conversions, J. Catal., 251 (1), 21–27.

[4] Pastvova, J., Kaucky, D., Moravkova, J., Rathousky, J., Sklenak, S., Vorokhta, M., Brabec, L., Pilar, R., Jakubec, I., Tabor, E., Klein, P., and Sazama, P., 2017, Effect of enhanced accessibility of acid sites in micromesoporous mordenite zeolites on hydroisomerization of n‑hexane, ACS Catal., 7 (9), 5781–5795.

[5] Chaouati, N., Soualah, A., Hussein, I., Comparot, J.D., and Pinard, L., 2016, Formation of weak and strong Brønsted acid sites during alkaline treatment on MOR zeolite, Appl. Catal., A, 526, 95–104.

[6] Chen, C.Y., Ouyang, X., Zones, S.I., Banach, S.A., Elomari, S.A., Davis, T.M., and Ojo, A.F., 2012, Characterization of shape selective properties of zeolites via hydroisomerization of n-hexane, Microporous Mesoporous Mater., 164, 71–81.

[7] Baran, R., Millot, Y., Onfroy, T., Krafft, J.M., and Dzwigaj, S., 2012, Influence of the nitric acid treatment on Al removal, framework composition and acidity of BEA zeolite investigated by XRD, FTIR and NMR, Microporous Mesoporous Mater., 163, 122–130.

[8] Chung, K.W., 2008, Dealumination of mordenites with acetic acid and their catalytic activity in the alkylation of cumene, Microporous Mesoporous Mater., 11 (1-3), 544–550.

[9] Yusniyanti, F., 2018, Acid-alkaline treatment of mordenite as MoO3 support and its catalytic activity on the hydrotreatment of cellulose-derived bio-oil, Thesis, Department of Chemistry, Universitas Gadjah Mada, Yogyakarta.

[10] Ong, L.H., Dömök, M., Olindo, R., van Veen, A.C., and Lercher, J.A., 2012, Dealumination of HZSM-5 via steam-treatment, Microporous Mesoporous Mater., 164, 9–20.

[11] Verboekend, D., Vilé, G., and Pérez-Ramírez, J., 2012, Hierarchical Y and USY zeolites designed by post-synthetic strategies, Adv. Funct. Mater., 22 (5), 916–928.

[12] Ahmed, M.H.M., Muraza, O., Yoshioka, M., and Yokoi, T., 2017, Effect of multi-step desilication and dealumination treatments on the performance of hierarchical EU-1 zeolite for converting methanol to olefins, Microporous Mesoporous Mater., 241, 79–88.

[13] Boveri, M., Márquez-Álvarez, C., Laborde, M.Á., and Sastre, E., 2006, Steam and acid dealumination of mordenite Characterization and influence on the catalytic performance in linear alkylbenzene synthesis, Catal. Today, 114 (2-3), 217–225.

[14] Stefanidis, S., Kalogiannis, K., Iliopoulou, E.F., Lappas, A.A., Triguero, J.M., Navarro, M.T., Chica, A., and Rey, F., 2013, Mesopore-modified mordenites as catalysts for catalytic pyrolysis of biomass and cracking of vacuum gasoil processes, Green Chem., 15 (6), 1647–1658.

[15] Silaghi, M.C., Chizallet, C., and Raybaud, P., 2014, Challenges on molecular aspects of dealumination and desilication of zeolites, Microporous Mesoporous Mater., 191, 82–96.

[16] Almutairi, S.M.T., Mezari, B., Filonenko, G.A., Magusin, P.C.M.M., Rigutto, M.S., Pidko, E.A., and Hensen, E.J.M., 2013, Influence of extraframework aluminum on the Brønsted acidity and catalytic reactivity of faujasite zeolite, ChemCatChem, 5, 452–466.

[17] Li, J., Li, X., Zhou, G., Wang, W., Wang, C., Komarneni, S., and Wang, Y., 2014, Catalytic fast pyrolysis of biomass with mesoporous ZSM-5 zeolites prepared by desilication with NaOH solutions, Appl. Catal., A, 470, 115–122.

[18] Bertrand-Drira, C., Cheng, X., Cacciaguerra, T., Trens, P., Melinte, G., Ersen, O., Minoux, D., Finiels, A., Fajula, F., and Gerardin, C., 2014, Mesoporous mordenites obtained by desilication: Mechanistic considerations and evaluation in catalytic oligomerization of pentene, Microporous Mesoporous Mater., 213, 142–149.

[19] Gackowski, M., Tarach, K., Kuterasiński, Ł., Podobiński, J., Jarczewski, S., Kuśtrowski, P., and Datka, J., 2018, Hierarchical zeolites Y obtained by desilication: Porosity, acidity and catalytic properties, Microporous Mesoporous Mater., 263, 282–288.

[20] Sandoval-Díaz, L.-E., González-Amaya, J.-A., and Trujillo, C.-A., 2015, General aspects of zeolite acidity characterization, Microporous Mesoporous Mater., 215, 229–243.

[21] Agudelo, J.L., Hensen, E.J.M., Giraldo, S.A., and Hoyos, L.J., 2015, Influence of steam-calcination and acid leaching treatment on the VGO hydrocracking performance of faujasite zeolite, Fuel Process. Technol., 133, 89–96.

[22] Kruk, M., and Jaroniec, M., 2001, Gas adsorption characterization of ordered organic-inorganic nanocomposite materials, Chem. Mater., 13 (10), 3169–3183.

[23] Silvestre-Albero, A.M., Juárez-Galán, J.M., Silvestre-Albero, J., and Rodríguez-Reinoso, F., 2012, Low-pressure hysteresis in adsorption: An artifact?, J. Phys. Chem. C, 116 (31), 16652–16655.

[24] Vu, X.H., Eckelt, R., Armbruster, U., and Martin, A., 2014, High-temperature synthesis of ordered mesoporous aluminosilicates from ZSM-5 nanoseeds with improved acidic properties, Nanomaterials, 4 (3), 712–725.

[25] Góra-Marek, K., Tarach, K., Tekla, J., Olejniczak, Z., Kus̈trowski, P., Liu, L., Martinez-Triguero, J., and Rey, F., 2014, Hierarchical mordenite dedicated to the fluid catalytic cracking process: Catalytic performance regarding textural and acidic properties, J. Phys. Chem. C, 118 (48), 28043–28054.



DOI: https://doi.org/10.22146/ijc.51496

Article Metrics

Abstract views : 2537 | views : 2914


Copyright (c) 2020 Indonesian Journal of Chemistry

Creative Commons License
This work is licensed under a Creative Commons Attribution-NonCommercial-NoDerivatives 4.0 International License.

 


Indonesian Journal of Chemistry (ISSN 1411-9420 /e-ISSN 2460-1578) - Chemistry Department, Universitas Gadjah Mada, Indonesia.

Web
Analytics View The Statistics of Indones. J. Chem.