Abstract
The catalytic properties of materials based on terbium-doped and nickel-modified mesoporous silica gels prepared by the high-temperature template method were studied. The surface morphology and textural characteristics of the obtained samples were studied by scanning electron microscopy, X-ray phase analysis, and inductively coupled plasma mass spectrometry. The catalytic activity of the obtained catalysts was studied in the hydrogenation reaction of benzene, m-, p-, and o-xylene in the temperature range of 80–170°C and at a hydrogen pressure of 3 atm. It was established that doping with terbium leads to an increase in the catalytic activity of the catalyst modified with nickel in the hydrogenation reaction of benzene derivatives. Therefore, it was shown that mesoporous silica gel doped with terbium and modified with nickel is an effective catalyst for the hydrogenation of benzene and xylenes.
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REFERENCES
Zhang, J., Ma, Y., Shi, F., Liu, L., and Deng, Y., Room temperature ionic liquids as templates in the synthesis of mesoporous silica via a sol–gel method, Micropor. Mesopor. Mater., 2009, vol. 119, nos. 1–3, pp. 97–103. https://doi.org/10.1016/j.micromeso.2008.10.003
Wu, S.H., Mou, C.Y., and Lin, H.P., Synthesis of mesoporous silica nanoparticles, Chem. Soc. Rev., 2013, vol. 42, no. 9, pp. 3862–3875. https://doi.org/10.1039/C3CS35405A
Rahman, N.A., Widhiana, I., Juliastuti, S.R., and Setyawan, H., Synthesis of mesoporous silica with controlled pore structure from bagasse ash as a silica source, Colloids Surf. A Physicochem. Eng. Asp., 2015, vol. 476, pp. 1–7. https://doi.org/10.1016/j.colsurfa.2015.03.018
Li, B., Shu, D., Wang, R., Zhai, L., Chai, Y., Lan, Y., Cao, H., and Zou, C., Polyethylene glycol/silica (PEG@SiO2) composite inspired by the synthesis of mesoporous materials as shape-stabilized phase change material for energy storage, Renew. Energy, 2020, vol. 145, pp. 84–92. https://doi.org/10.1016/j.renene.2019.05.118
Kaur, A., Bajaj, B., Kaushik, A., Saini, A., and Sud, D., A review on template assisted synthesis of multi-functional metal oxide nanostructures: Status and prospects, Mater. Sci. Eng. B, 2022, vol. 286, p. 116005. https://doi.org/10.1016/j.mseb.2022.116005
Yu, X. and Williams, C.T., Recent advances in the applications of mesoporous silica in heterogeneous catalysis, Catal. Sci. Technol., 2022, vol. 1219, pp. 5765–5794. https://doi.org/10.1039/D2CY00001F
Yi, C., Zhang, L., Xiang, G., and Liu, Z., Size effect of Co–N–C-functionalized mesoporous silica hollow nanoreactors on the catalytic performance for the selective oxidation of ethylbenzene, New J. Chem., 2022, vol. 46, no. 31, pp. 15102–15109. https://doi.org/10.1039/D2NJ01705A
Uruş, S., Microwave assisted catalytic oxidation of cyclohexene, cyclohexane, cyclooctane and styrene with metal complexes of bis (azo-imine) ligands supported on mesoporous silica, Phosphorus Sulfur Silicon Relat. Elem., 2022, vol. 197, no. 8, pp. 799–809. https://doi.org/10.1080/10426507.2022.2031196
Chi, Y.S., Lin, H.P., and Mou, C.Y., CO oxidation over gold nanocatalyst confined in mesoporous silica, Appl. Catal. A, 2005, vol. 284, nos. 1–2, pp. 199–206. https://doi.org/10.1016/j.apcata.2005.01.034
Al Soubaihi, R.M., Saoud, K.M., Ye, F., Myint, M.T.Z., Saeed, S., and Dutta, J., Synthesis of hierarchically porous silica aerogel supported palladium catalyst for low-temperature CO oxidation under ignition/extinction conditions, Micropor. Mesopor. Mater., 2020, vol. 292, p. 109758. https://doi.org/10.1016/j.micromeso.2019.109758
Tokranova, E.O., Tokranov, A.A., Vinogradov, K.Yu., Shafigulin, R.V., and Bulanova, A.V., Mesoporous silica gel doped with dysprosium and modified with copper: A selective catalyst for the hydrogenation of 1-hexyne/1-hexene mixture, Int. J. Chem. Kinetics, 2022, vol. 54, no. 11, pp. 647–658. https://doi.org/10.1002/kin.21602
Yang, Y., Xu, B., He, J., Shi, J., Yu, L., and Fan, Y., Magnetically separable mesoporous silica-supported palladium nanoparticle-catalyzed selective hydrogenation of naphthalene to tetralin, Appl. Organomet. Chem., 2019, vol. 33, no. 11, p. e5204. https://doi.org/10.1002/aoc.5204
Mihalcik, D.J. and Lin, W., Mesoporous silica nanosphere-supported chiral ruthenium catalysts: synthesis, characterization, and asymmetric hydrogenation studies, ChemCatChem, 2009, vol. 1, no. 3, pp. 406–413. https://doi.org/10.1002/cctc200900188
Lo, H.K., Thiel, I., and Copéret, C., Efficient CO2 hydrogenation to formate with immobilized Ir-catalysts based on mesoporous silica beads, Chem. A Eur. J., 2019, vol. 25, no. 40, pp. 9443–9446. https://doi.org/10.1002/chem.201901663
Wang, H.M., Chen, Y., Yan, X., Lang, W.Z., and Guo, Y.J., Cr doped mesoporous silica spheres for propane dehydrogenation in the presence of CO2: Effect of Cr adding time in sol–gel process, Micropor. Mesopor. Mater., 2019, vol. 284, pp. 69–77. https://doi.org/10.1016/j.micromeso.2019.04.016
Samanta, P.K., Ray, S., Das, T., Gage, S.H., Nandi, M., Richards, R.M., and Biswas, P., Palladium oxide nanoparticles intercalated mesoporous silica for solvent free acceptorless dehydrogenation reactions of alcohols, Micropor. Mesopor. Mater., 2019, vol. 284, pp. 186–197. https://doi.org/10.1016/j.micromeso.2019.04.034
Finger, P.H., Osmari, T.A., Cabral, N.M., Bueno, J.M.C., and Gallo, J.M.R., Direct synthesis of Cu supported on mesoporous silica: Tailoring the Cu loading and the activity for ethanol dehydrogenation, Catal. Today, 2021, vol. 381, pp. 26–33. https://doi.org/10.1016/j.cattod.2020.10.019
Bai, X., Lin, C., Wang, Y., Ma, J., Wang, X., Yao, X., and Tang, B., Preparation of Zn doped mesoporous silica nanoparticles (Zn–MSNs) for the improvement of mechanical and antibacterial properties of dental resin composites, Dent. Mater., 2020, vol. 36, no. 6, pp. 794–807. https://doi.org/10.1016/j.dental.2020.03.026
Malhotra, R. and Ali, A., 5-Na/ZnO doped mesoporous silica as reusable solid catalyst for biodiesel production via transesterification of virgin cottonseed oil, Renew. Energy, 2019, vol. 133, pp. 606–619. https://doi.org/10.1016/j.renene.2018.10.055
EL-Mahdy, A.F.M., Yu, T.C., and Kuo, S.W., Synthesis of multiple heteroatom-doped mesoporous carbon/silica composites for supercapacitors, Chem. Eng. J., 2021, vol. 414, p. 128796. https://doi.org/10.1016/j.cej.2021.128796
Wu, Y.L., Han, Z.F., Yan, X., Lang, W.Z., and Guo, Y.J., Effective synthesis of vanadium-doped mesoporous silica nanospheres by sol–gel method for propane dehydrogenation reaction, Micropor. Mesopor. Mater., 2022, vol. 330, p. 111616. https://doi.org/10.1016/j.micromeso.2021.111616
Zheng, B., Fan, J., Chen, B., Qin, X., Wang, J., Wang, F., Den R., and Liu, X., Rare-earth doping in nanostructured inorganic materials, Chem. Rev., 2022, vol. 122, no. 6, pp. 5519–5603. https://doi.org/10.1021/acs.chemrev.1c00644
Sibu, C.P., Kumar, S.R., Mukundan, P., and Warrier, K.G.K., Structural modifications and associated properties of lanthanum oxide doped sol–gel nanosized titanium oxide, Chem. Mater., 2002, vol. 14, no. 7, pp. 2876–2881. https://doi.org/10.1021/cm010966p
Zykin, M.A., Dyakonov, A.K., Eliseev, A.A., Trusov, L.A., Kremer, R.K., Dinnebier, R.E., Jansen, M., and Kazin, P.E., Tb-based silicate apatites showing slow magnetization relaxation with identical parameters for the Tb3+ and Dy3+ counter ions, RSC Adv., 2021, vol. 11, no. 12, pp. 6926–6933. https://doi.org/10.1039/D1RA00613D
Speight, J.G., Production, properties and environmental impact of hydrocarbon fuel conversion, Advances in Clean Hydrocarbon Fuel Processing, Woodhead Publishing, 2011, pp. 54–82. https://doi.org/10.1533/9780857093783.1.54
Pan, H.B. and Wai, C.M., One-step synthesis of size-tunable rhodium nanoparticles on carbon nanotubes: a study of particle size effect on hydrogenation of xylene, J. Phys. Chem. C, 2010, vol. 114, no. 26, pp. 11364–11369. https://doi.org/10.1021/jp101368p
Keane, M.A. (). The Hydrogenation of o-, m-, and p-xylene over Ni/SiO2, J. Catal., 1997, vol. 166, no. 2, pp. 347–355. https://doi.org/10.1006/jcat.1997.1527
Filippova, E.O., Shafigulin, R.V., and Bulanova, A.V., Kinetic characteristics of catalysts based on mesoporous silica gel doped with Dy and modified with Ni, Cu, Ag, in hydrogenation of xylenes, Russ. J. Phys. Chem. A, 2021, vol. 95, no. 4, pp. 690–695. https://doi.org/10.1134/S0036024421040051
Toppinen, S., Rantakylä, T.K., Salmi, T., and Aittamaa, J., Kinetics of the liquid phase hydrogenation of di-and trisubstituted alkylbenzenes over a nickel catalyst, Ind. Eng. Chem. Res., 1996, vol. 35, no. 12, pp. 4424–4433. https://doi.org/10.1021/ie950636c
Mittendorfer, F. and Hafner, J., Hydrogenation of benzene on Ni (111) – a DFT study, J. Phys. Chem. B, 2002, vol. 106, no. 51, pp. 13299–13305. https://doi.org/10.1021/jp026010z
Wojcieszak, R., Monteverdi, S., Mercy, M., Nowak, I., Ziolek, M., and Bettahar, M.M., Nickel containing MCM-41 and AlMCM-41 mesoporous molecular sieves: Characteristics and activity in the hydrogenation of benzene, Appl. Catal. A, 2004, vol. 268, nos. 1–2, pp. 241–253. https://doi.org/10.1016/j.apcata.2004.03.047
Keypour, H. and Noroozi, M., Hydrogenation of benzene in gasoline fuel over nanoparticles (Ni, Pt, Pd, Ru and Rh) supported fullerene: Comparison study, J. Appl. Chem., 2016, vol. 10, no. 37, pp. 31–42. https://doi.org/10.22075/CHEM.2017.718
Wojcieszak, R., Jasik, A., Monteverdi, S., Ziolek, M., and Bettahar, M.M., Nickel niobia interaction in non-classical Ni/Nb2O5 catalysts, J. Mol. Catal. A Chem., 2006, vol. 256, nos. 1–2, pp. 225–233. https://doi.org/10.1016/j.molcata.2006.04.053
Wang, W., High nickel- and titania-containing mesoporous silicas: synthesis and characterization, Doctoral Dissertation, Loughborough University, 2005.
Barrio, V.L., Arias, P.L., Cambra, J.F., Güemez, M.B., Pawelec, B., and Fierro, J.L.G., Aromatics hydrogenation on silica–alumina supported palladium–nickel catalysts, Appl. Catal. A, 2003, vol. 242, no. 1, pp. 17–30. https://doi.org/10.1016/S0926-860X(02)00489-1
Pawelec, B., Castano, P., Arandes, J. M., Bilbao, J., Thomas, S., Peña, M.A., and Fierro, J.L.G., Factors influencing the thioresistance of nickel catalysts in aromatics hydrogenation, Appl. Catal. A, 2007, vol. 317, no. 1, pp. 20–33. https://doi.org/10.1016/j.apcata.2006.09.035
Barrio, V.L., Arias, P.L., Cambra, J.F., Güemez, M.B., Pawelec, B., and Fierro, J.L.G., Modification of the Pd/SiO2–Al2O3 catalyst’s thioresistance by the addition of a second metal (Pt, Ru, and Ni), Catal. Commun., 2004, vol. 5, no. 4, pp. 173–178. https://doi.org/10.1016/j.catcom.2004.01.004
Louloudi, A. and Papayannakos, N., Hydrogenation of benzene on Ni/Al-pillared montmorillonite catalysts, Appl. Catal. A, 2000, vol. 204, no. 1, pp. 167–176. https://doi.org/10.1016/S0926-860X(00)00516-0
Uttamaprakrom, W., Reubroycharoen, P., Charoensiritanasin, P., Tatiyapantarak, J., Srifa, A., Koo-Amornpattana, W., Chaiwat, W., Sakdaronnarong C., and Ratchahat, S., Development of Ni–Ce/Al–MCM-41 catalysts prepared from natural kaolin for CO2 methanation, J. Environ. Chem. Eng., 2021, vol. 9, no. 5, p. 106150. https://doi.org/10.1016/j.jece.2021.106150
Spennati, E., Riani, P., and Garbarino, G., A perspective of lanthanide promoted Ni-catalysts for CO2 hydrogenation to methane: catalytic activity and open challenges, Catal. Today, 2023, vol. 418, p. 114131. https://doi.org/10.1016/j.cattod.2023.114131
Shafigulin, R.V., Filippova, E.O., Shmelev, A.A., and Bulanova, A.V., Mesoporous silica doped with dysprosium and modified with nickel: a highly efficient and heterogeneous catalyst for the hydrogenation of benzene, ethylbenzene and xylenes, Catal. Lett., 2019, vol. 149, pp. 916–928. https://doi.org/10.1007/s10562-019-02678-x
IUPAC Compendium of Chemical Terminology. Version 2.3.2. 2012-08-19. http://www.iupac.org/.
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Tokranov, A.A., Tokranova, E.O., Shafigulin, R.V. et al. Catalyst Based on Mesoporous Silica Gel Doped with Terbium and Modified with Nickel Obtained by High-Temperature Template Method for Aromatic Hydrocarbons Hydrogenation. Int. J Self-Propag. High-Temp. Synth. 33, 49–57 (2024). https://doi.org/10.3103/S1061386224010096
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DOI: https://doi.org/10.3103/S1061386224010096