Performance of a Hybrid Catalyst from Amine Groups and Nickel Nanoparticles Immobilized on Lapindo Mud in Selective Production of Bio-hydrocarbons

Wega Trisunaryanti(1*), Salma Nur Azizah(2), Dyah Ayu Fatmawati(3), Triyono Triyono(4), Novia Cahya Ningrum(5)

(1) Department of Chemistry, Faculty of Mathematics and Natural Sciences, Universitas Gadjah Mada, Sekip Utara, Yogyakarta 55281, 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
(4) Department of Chemistry, Faculty of Mathematics and Natural Sciences, Universitas Gadjah Mada, Sekip Utara, Yogyakarta 55281, Indonesia
(5) Department of Chemistry, Faculty of Mathematics and Natural Sciences, Universitas Gadjah Mada, Sekip Utara, Yogyakarta 55281, Indonesia
(*) Corresponding Author


In the present work, optimum conditions for hydrocracking of waste palm cooking oil (WPCO) over a Ni-NH2/Lapindo mud catalyst were studied to obtain a high quantity and quality of biofuel. The utilized catalyst support material was Lapindo mud (LM) from Sidoarjo, Indonesia, which was only given physical treatment (i.e., washing, drying, grinding, and calcining). Ni/LM was prepared via wet impregnation in three different Ni weight loadings: 1, 5, and 10 wt.%, which were denoted as Ni(A)/LM, Ni(B)/LM, and Ni(C)/LM, respectively. As a result, the hydrocracking test of WPCO under the temperature of 470 °C and a feed/catalyst weight ratio of 50 showed that the Ni(A)/LM catalyst produced the highest liquid product reaching 46.65 wt.% among the other Ni-based catalysts. The liquid product can be increased drastically to 63.93 wt.% under a more optimum temperature at 550 °C. Functionalization of Ni(A)/LM as the best catalyst was carried out by grafting method with NH2 groups from 3-APTMS, resulting in Ni(A)-NH2/LM. This modification increased the liquid product to 68.17 wt.% under hydrocracking conditions using a weight ratio of 75. Moreover, the reusability of Ni(A)-NH2/LM was found to be effective for three hydrocracking runs, constantly yielding an average biofuel of 80 wt.%.


hydrocracking; Lapindo mud; nickel; 3-APTMS; waste palm cooking oil

Full Text:

Full Text PDF


[1] Kusumastuti, H., Trisunaryanti, W., Falah, I.I., and Marsuki, M.F., 2018, Synthesis of mesoporous silica-alumina from lapindo mud as a support of Ni and Mo metals catalysts for hydrocracking of pyrolyzed α-cellulose, Rasayan J. Chem., 11 (2), 522–530.

[2] Vazquez, N.I., Gonzalez, Z., Ferrari, B., and Castro, Y., 2017, Synthesis of mesoporous silica nanoparticles by sol-gel as nanocontainer for future drug delivery applications, Bol. Soc. Esp. Ceram. Vidrio, 56 (3), 139–145.

[3] Niculescu, V.C., 2020, Mesoporous silica nanoparticles for bio-applications, Front. Mater., 7, 36.

[4] Rizzi, F., Castaldo, R., Latronico, T., Lasala, P., Gentile, G., Lavorgna, M., Striccoli, M., Agostiano, A., Comparelli, R., Depalo, N., Curri, M.L., and Fanizza, E., 2021, High surface area mesoporous silica nanoparticles with tunable size in the sub-micrometer regime: Insights on the size and porosity control mechanisms, Molecules, 26 (14), 4247.

[5] Lin, Y.S., Hurley, K.R., and Haynes, C.L., 2012, Critical considerations in the biomedical use of mesoporous silica nanoparticles, J. Phys. Chem. Lett., 3 (3), 364–374.)

[6] Kumar, S., Malik, M.M., and Purohit, R., 2017, Synthesis methods of mesoporous silica materials, Mater. Today: Proc., 4 (2), 350–357.

[7] Trisunaryanti, W., Larasati, S., Bahri, S., Ni’mah, Y.L., Efiyanti, L., Amri, K., Nuryanto, R., and Sumbogo, S.D., 2020, Performance comparison of Ni-Fe loaded on NH2-functionalized mesoporous silica and beach sand in the hydrotreatment of waste palm cooking oil, J. Environ. Chem. Eng., 8 (6), 104477.

[8] Trisunaryanti, W., Triyono, Paramesti, C., Larasati, S., Santoso, N.R., and Fatmawati, D.A., 2020, Synthesis and characterization of Ni-NH2/mesoporous silica catalyst from Lapindo mud for hydrocracking of waste cooking oil into biofuel, Rasayan J. Chem., 13, 1386–1393.

[9] Li, G., Chen, L., Fan, R., Liu, D., Chen, S., Li, X., and Chung, K.H., 2019, Catalytic deoxygenation of C 18 fatty acid over supported metal Ni catalysts promoted by the basic sites of ZnAl2O4 spinel phase, Catal. Sci. Technol., 9 (1), 213–222.

[10] Jang, M.S., Phan, T.N., Chung, I.S., Lee, I.G., Park, Y.K., and Ko, C.H., 2018, Metallic nickel supported on mesoporous silica as catalyst for hydrodeoxygenation: Effect of pore size and structure, Res. Chem. Intermed., 44 (6), 3723–3735.

[11] Paramesti, C., Trisunaryanti, W., Sudiono, S., Triyono, T., Larasati, S., Santoso, N.R., and Fatmawati, D.A., 2021, The influence of metal loading amount on Ni/mesoporous silica extracted from Lapindo mud templated by CTAB for conversion of waste cooking oil into biofuel, Bull. Chem. React. Eng. Catal., 16 (1), 22–30.

[12] Lu, H.T., 2013, Synthesis and characterization of amino-functionalized silica nanoparticles, Colloid J., 75 (3), 311–318.

[13] Ma, Y., Wu, Y., Lee, J.G., He, L., Rother, G., Fameau, A.L., Shelton, W.A., and Bharti, B., 2020, Adsorption of fatty acid molecules on amine-functionalized silica nanoparticles: Surface organization and foam stability, Langmuir, 36 (14), 3703–3712.

[14] Kandel, K., Frederickson, C., Smith, E.A., Lee, Y.J., and Slowing, I.I., 2013, Bifunctional adsorbent-catalytic nanoparticles for the refining of renewable feedstocks, ACS Catal., 3, 2750–2758.

[15] Chuah, L.F., Mohd Salleh, N.H., Osnin, N.A., Alcaide, J.I., Abdul Majid, M.H., Abdullah, A.A., Bokhari, A., A Jalil, E.E., and Klemeš, J.J., 2021, Profiling Malaysian ship registration and seafarers for streamlining future Malaysian shipping governance, Aust. J. Marit. Ocean Aff., 13 (4), 225–261.

[16] Nanda, S., Rana, R., Hunter, H.N., Fang, Z., Dalai, A.K., and Kozinski, J.A., 2019, Hydrothermal catalytic processing of waste cooking oil for hydrogen-rich syngas production, Chem. Eng. Sci., 195, 935–945.

[17] Ong, A.S.H., and Goh, S.H., 2002, Palm oil: A healthful and cost-effective dietary component, Food Nutr. Bull., 23 (1), 11–22.

[18] Hartono, Z.A., and Cahyono, B., 2020, Effect of using B30 palm oil biodiesel to deposit forming and wear metal of diesel engine components, Int. J. Mar. Eng. Innovation Res., 5 (1), 10–19.

[19] Ayetor, G.K., Sunnu, A., and Parbey, J., 2015, Effect of biodiesel production parameters on viscosity and yield of methyl esters: Jatropha curcas, Elaeis guineensis and Cocos nucifera, Alexandria Eng. J., 54, 1285–1290.

[20] Goswami, G., Bora, R., and Rathore, M.S., 2016, Oxidation of cooking oils due to repeated frying and human health, Int. J. Sci. Technol. Manage., 4 (1), 495–501.

[21] Huang, D., Zhou, H., and Lin, L., 2012, Biodiesel: An alternative to conventional fuel, Energy Procedia, 16, 1874–1885.

[22] Murachman, B., Deendarlianto, D., Nissaraly, H.F., and Hasyim, W., 2014, Experimental study on hydrocracking process of asbuton hydrocarbon based on the aromatic, and waxy residue based on paraffinic, by using Pt/Pd and γ-alumina catalyst in a fixed bed reactor, ASEAN J. Chem. Eng., 14 (1), 59–75.

[23] Treese, S.A., Pujadó, P.R., and Jones, D.S.J., 2015, Handbook of Petroleum Processing, Springer, Cham, Switzerland.

[24] Alkhaldi, S., and Husein, M.M., 2014, Hydrocracking of heavy oil by means of in situ prepared ultradispersed nickel nanocatalyst, Energy Fuels, 28 (1), 643–649.

[25] Khoiri, H.M., Trisunaryanti, W., and Dewi, K., 2015, Synthesis of NH2/MCM-41 catalysts using silica of Sidoarjo mud and their characterization for palm oil transesterification, IOSR J. Appl. Chem., 8 (8), 50–56.

[26] Nugrahaningtyas, K.D., Trisunaryanti, W., Triyono, T., Nuryono, N., Widjonarko, D.M., Yusnani, A., and Mulyani, M., 2009, Preparation and characterization the non-sulfided metal catalyst: Ni/USY and NiMo/USY, Indones. J. Chem., 9 (2), 177–183.

[27] Kefaifi, A., Sahraoui, T., Kheloufi, A., and Drouiche, N., 2018, Silica sand etching behavior during leaching process using design of experiments method (DOE), Silicon, 10 (3), 1187–1193.

[28] Dubey, R.S., Rajesh, Y.B.R.D., and More, M.A., 2015, Synthesis and characterization of SiO2 nanoparticles via sol-gel method for industrial applications, Mater. Today: Proc., 2 (4-5), 3575–3579.

[29] Li, X., Han, C., Zhu, W., Ma, W., Luo, Y., Zhou, Y., Yu, J., and Wei, K., 2014, Cr(VI) removal from aqueous by adsorption on amine-functionalized mesoporous silica prepared from silica fume, J. Chem., 2014, 765856.

[30] Oliveira, D.M., and Andrada, A.S., 2019, Synthesis of ordered mesoporous silica MCM-41 with controlled morphology for potential application in controlled drug delivery systems, Cerâmica, 65, 170–179.

[31] Cychosz, K.A., and Thommes, M., 2018, Progress in the physisorption characterization of nanoporous gas storage materials, Engineering, 4 (4), 559–566.

[32] Thommes, M., Kaneko, K., Neimark, A.V., Olivier, J.P., Rodriguez-Reinoso, F., Rouquerol, J., and Sing, K.S.W., 2015, Physisorption of gases, with special reference to the evaluation of surface area and pore size distribution (IUPAC Technical Report), Pure Appl. Chem., 87 (9-10), 1051–1069.

[33] Trisunaryanti, W., Wijaya, K., Triyono, T., Adriani, A.R., and Larasati, S., 2021, Green synthesis of hierarchical porous carbon prepared from coconut lumber sawdust as Ni-based catalyst support for hydrotreating Callophyllum inophyllum oil, Results Eng., 11, 100258.

[34] Qi, L., Tang, X., Wang, Z., and Peng, X., 2017, Pore characterization of different types of coal from coal and gas outburst disaster sites using low temperature nitrogen adsorption approach, Int. J. Min. Sci. Technol., 27 (2), 371–377.

[35] Junaidi, R., Hasan, A., and Zamhari, M., 2019, Influence the addition of Lapindo mud is calcined to the quality of cement podzoland by using electric furnace, J. Phys.: Conf. Ser., 1167, 012043.

[36] Hu, H., Lu, S., Li, T., Zhang, Y., Guo, C., Zhu, H., Jin, Y., Du, M., and Zhang, W., 2021, Controlled growth of ultrafine metal nanoparticles mediated by solid supports, Nanoscale Adv., 3 (7), 1865–1886.

[37] Ochoa-Hernández, C., Yang, Y., Pizarro, P., de La Peña O’Shea, V.A., Coronado, J.M., and Serrano, D.P., 2013, Hydrocarbons production through hydrotreating of methyl esters over Ni and Co supported on SBA-15 and Al-SBA-15, Catal. Today, 210, 81–88.

[38] Auepattana-aumrung, C., Márquez, V., Wannakao, S., Jongsomjit, B., Panpranot, J., and Praserthdam, P., 2020, Role of Al in Na-ZSM-5 zeolite structure on catalyst stability in butene cracking reaction, Sci. Rep., 10 (1), 13643.

[39] Anderson, J.E., Dicicco, D.M., Ginder, J.M., Kramer, U., Leone, T.G., Raney-Pablo, H.E., and Wallington, T.J., 2012, High octane number ethanol-gasoline blends: Quantifying the potential benefits in the United States, Fuel, 97, 585–594.

[40] Kubička, D., and Kaluža, L., 2010, Deoxygenation of vegetable oils over sulfided Ni, Mo and NiMo catalysts, Appl. Catal., A, 372 (2), 199–208.


Article Metrics

Abstract views : 2453 | views : 1731

Copyright (c) 2022 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.

Analytics View The Statistics of Indones. J. Chem.