International Journal of Environment and Bioenergy, 2012, 3(3): International Journal of Environment and Bioenergy

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1 International Journal of Environment and Bioenergy, 2012, 3(3): International Journal of Environment and Bioenergy Journal homepage: ISSN: Florida, USA Article Bio-gasoline from Catalytic Hydrocracking Reaction of Waste Cooking Oil Using Bayah Natural Zeolite E.N. Rohmah 1, *, A.Rochmat 1, S.D. Sumbogo 2 1 Department of Chemical Engineering, University of Sultan Ageng Tirtayasa, Cilegon, Indonesia 2 BEnergy Technology Center (BBTE), Agency for the Assessment and Application of Technology (BPPT), Serpong, Indonesia * Author to whom correspondence should be addressed; elfinurrohmah@gmail.com. Article history: Received 12 June 2012, Received in revised form 7 August 2012, Accepted 8 August 2012, Published 29 August Abstract: Production of bio-gasoline through catalytic hydrocracking of waste cooking oil was carried out in a 1.0 L autoclave. The reaction conditions were varied at temperatures of o C, initial hydrogen pressure of 8 Mpa, for 60 and 90 min. of reaction time. Bayah natural zeolite was applied as catalyst for converting waste cooking oil to biogasoline. The highest yield of bio-gasoline was obtained at temperature of 400 o C with different amount of catalyst. The influence of reaction conditions to the yield and characteristic of product were discussed in this study. Keywords: bio-gasoline, waste cooking oil, catalytic hydrocracking, Bayah natural zeolite. 1. Introduction Global warming caused by burning fossil energy sources continues to increase with increases in energy use for subsistence. Fossil energy sources have a limited amount of reserves and decreases yearly. Continuoud exploitation of fossil energy resources will damage the provition of energy souces to meet energy need in the future. To prevent occurrence of energy sources shortages, the substitute energy sources such as from plants, wind, water, etc must be found in the suitable amount. Transportation sector in Indonesia is one of the biggest sector that much consume fossil fuel. According to Indonesia Energy Outlook 2010, energy demand in the transportation sector increased at a rate of growth of 4.1% yearly. A very rapid rate of growth will be extremely burdensome supply of

2 202 fuel oil derived from petroleum and will further enhance the negative effects of burning fossil fuels. Indonesia is a big country that rich in energy resources. Indonesia can utilize renewable energy such as bio-fuels for the substitution of conventional fossil fuel. Palm plantation in Indonesia produces abundantly of crude palm oil that can be derived to cooking oil and other product such soap, cosmetics etc. The use of cooking oil will produce much waste cooking oil (WCO) that still able to be processed and converted to bio-fuel. Some researcher have conducted an exellent chalengest to convert WCO to bio-diesel. Farouq et al. (2005) reported a liquid hydrocarbon fuels from palm oil by catalytic cracking over aluminosilicate mesoporous catalyst with various Si/Al ratios, and claimed the conversion of palm oil was 80 90% wt. Pramila et al. (2006) reported a catalytic cracking of palm oil for the production of bio-fuel over REY catalyst in a transport riser reactor at atmospheric pressure. WCO that abundantly available is a bio-oil that contained triglycerides and it is a derivative of crude palm oil. Free fatty acid (FFA) in WCO is also similar with the FFA in crude palm oil (CPO) (Table 1), so it is possible to be processed for more valuable such as bio-fuel for vehicle and bio-lpg. In the present study, hydrocracking of WCO was carried out to produce bio-gasoline to subtitute fuel for vehicle from petroleum. Bayah natural zeolite was applied as catalyst in the hydrocracking reaction to increase the yield of bio-gasoline. Table 1. Characteristic of waste cooking oil compare to CPO Fatty Acid CPO WCO Miristic Palmitat Tearic Arachidic Behenic NA - Palmitoleic Oleat Margarat Stearat Linoleat Linolenic Sources: Gubitz et al., 1999; Sidjabat, Methods Bayah natural zeolite was applied as catalyst in this study. The catalyst was activated before apllying to the reaction. Bayah natural zeolite was crushed to pass 100 mesh and activated using sulfuric acid and dried in the oven at 110 o C for 15 h. Activated catalyst is then stored in desiccators to

3 203 avoid moisturizing. Activation was conducted to increase active site. Catalytic hydro-cracking of WCO over Bayah natural zeolite as catalyst was carried out in a 1 L autoclave (Fig. 1). Feed such as WCO and catalyst was loaded in the reactor where catalyst to WCO ratio was varied as 1:75 and 1:100, to investigate the effect of catalyst amount on converting WCO to bio-fuel. Leak test was conducted by loading hydrogen gas up to 15 MPa at room temperature and kept for 2 h per running to make sure that there is no leak during heating and reaction. Heating time for each condition was kept for 40 min by adjusting the temperature controller. The stiring speed was 500 rpm. Reaction time was measured after temperature reached to reaction condition. Reaction temperature was varied o C. Reaction was cooled down rapidly to room temperature after finishing reaction to minimize further reaction. The product of hydrocracking was collected, and liquid product was separated from catalyst by filtration. Figure 1. Flowchart of research.

4 204 Liquid product from hydrocracking of WCO was analyzed using GC-MS (GCMS-QP2010S SHIMADZU) and GC-FID (Yanaco, GC-2800) to identify and clarify the yield of bio-gasoline. 3. Results and Discussion 3.1. Conversion of Product Bayah natural zeolite was applied as catalyst in this study, and activation was conducted to increase active site (Table 2). Table 2. BET result of Bayah natural zeolite catalyst Parameter Before activation After activation Active site (m 2 /g) Liquid product from hydrocracking of WCO was analyzed using GC-MS, and Fig. 2 shows GC-MS chromatograms of bio-fuel product. The sharp of peaks are identified as aliphatic hydrocarbons such as C6, C7, C8 - C11 by comparing the fragmentasion of the cromatogram to the library of GC-MS. Further more the bio-fuel product was analyzed using GC-FID to determine biogasoline, and Fig. 3 shows the GC-FID chromatogram of bio-gasoline product. Yield of bio-gasoline was counted base on peak area in range of retention time, whereas bio-gasoline has retention time up to 20 min, and bio-diesel from to 40 min. Figure 2. GC-MS chromatogram of bio-fuel.

5 uv(x10,000) Chromatogram min Figure 3. GC-FID chromatogram of bio-fuel. Hydro-cracking reaction is an endothermic reaction, at higher temperature gave higher energy to break the C-C bonding of triglyceride resulting lighter hydrocarbon and gaseous. On hydrocracking WCO over Bayah natural zeolite catalyst, it was revealed that the higher the temperature the lower the bio-gasoline yields. Changing reaction temperature 20 o C from standard condition gave significant differences on yield bio-fuel. Fig. 4 shows the conversion of WCO on catalytic hydrocracking over Bayah natural zeolite to produce bio-fuel in different reaction temperature. At standard condition of 400 o C, 8 MPa initial H 2 pressure, 1:100 of catalyst to WCO ratio and 60 min reaction time, the yield of hydrocracking WCO was 91.07%. Decreasing reaction temperature of 20 o C from standard condition to 380 o C, the yield was increased slightly 2.49% to become 96.75%, but increasing reaction temperature to 420 o C, the yield was decreased markedly 3.65% to become 87.75%. Figure 4. Yield conversion in different temperature.

6 206 To investigate the influence of catalyst amount in the hycrocracking WCO over Bayah natural zeolite, ratio of catalyst to WCO was varied to be 1:100 and 1:75. The result was described in Fig. 5. Hydrocracking of WCO at standard reaction condition using catalyst to WCO ratio of 1:100 achieved 91.07% of bio-fuel yield. Increasing the amount of catalyst to be 1:75 of catalyst to WCO ratio resulted the increasing bio-gasoline product slightly 1.56 % to be 92.51% of yield. It means the more catalyst to be applied in the catalytic hydrocracking reaction of WCO, the active site in the reaction increased and resulted more feed to be crack become lighter product. However, increasing catalyst to WCO ratio from 1/100 to 1/75 gave only slightly increasing of bio-fuel product. Figure 5. Yield conversion in different catalyst to WCO ratio. Reaction time was prolong to investigate the influence of reaction time to yield of bio-fuel (Fig. 6). Prolong reaction time to 90 min slightly decreased the yield of bio-fuel. The longger reaction time resulted in vaporation of light fraction to become gas phase. Figure 6. Yield conversion in different reaction time.

7 Influence of Reaction Condition to Yield of Bio-gasoline Fig. 7 shows the influence of reaction temperature to the yield of bio-gasoline. Increasing reation temperature from 400 to 420 o C enhanced the yield of bio-gasoline slightly to 63.37%. Figure 7. Yield conversion of bio-gasoline in different temperature. The same phenomenon was occurred by extent the reaction time to 90 min. Yiels of biogasoline increased 6.30% to be 67.19% in Fig. 8. During the extention time, hydrocracking reaction continuously occurred, the heavier fraction of WCO was attacked by hydrogen and the C-C bonding was broken, which produced gaseous. The effect of catalyst to WCO ratio reveal the most extreme phenemonen compared to the previous condition as shown in the Fig. 9. Increasing catalyst to WCO ratio to 1/75 the bio-gasoline product increased 6.30 % to be %. It means that the more catalyst to be applied to the hydrocracking reaction the amount active site increase and the reaction occur intensively to crack the C-C bond of WCO producing. Figure 8. Yield conversion of bio-gasoline and biodiesel in different reaction time.

8 208 Figure 9. Yield conversion of bio-gasoline in different amount of catalyst. 4. Conclusions Waste cooking oil can be converted to bio-gasoline throught catalytic hydrocracking over Bayah natural zeolite as catalyst and resulted bio-gasoline more than 92%. The higher reaction temperature, the more catalyst applied and the longer reaction time produced more lighter fraction of bio-gasoline Acknowledgment We thank to the Laboratory of Coal Liquefaction - BPPT and DIKTI of facilities and cooperation. References Elfi, M. (2011). Hydrocracking of Waste Cooking Oil to Produce Biogasoline and Biodiesel. SISEST, Universitas Sriwijaya. Ginting, A. B. (2007). Karakterisasi Komposisi Kimia, Luas Permukaan Pori dan Sifat Termal dari Zeolit Bayah, Tasikmalaya, dan Lampung. BATAN, Serpong. Ketaren, S. (1986). Pengantar Teknologi Minyak dan Lemak Pangan. Penerbit Universitas Indonesia, Jakarta. Meng, X. H. (2008). Catalytic and Thermal Pyrolysis of Atmospheric Residu. American Chemical Society, Washington DC Nasikin, M. (2009). Biogasoline from Palm Oil by Simultaneous Cracking and Hydrogenation

9 209 Reaction over Nimo/Zeolite Catalyst. Jurnal Penelitian Sains, Depok: Teknik Kimia FTUI. Nurjannah, I., and Achmad, R. D. D. (2008). Perengkahan Katalitik Asam Oleat Untuk Menghasilkan Biofuel Menggunakan HZSM-5 Sintesis. Surabaya, Jurusan Teknik Kimia FTI ITS. Purawiardi, R. (1999). Karakteristik Zeolit Alam Asal Bayah, Sukabumi, Jawa Barat. Buletin IPT, Vol. 5, No. 1. Sidjabat, O. (2004). Pengolahan minyak goreng bekas menjadi Biodiesel. Lembaran Publikasi, LEMIGAS Jakarta. Sotelo, R. D. (2010). Production of Green Diesel by Hydrocracking of Canola Oil on Ni-Mo/γ-Al2O3 and Pt-Zeolitic Based Catalysts. Biomass Technology Research Center National Institute of Advanced Industrial Science and Technology, Japan, Chugoku, Hirosuehiro, Kure, Hiroshima. Twaiq, F. A., Zabidi, N. A., and Bhatia, S. (1999). Catalytic conversion of palm oil to hydrocarbons: Performance of various zeolite catalysts. Ind. Eng. Chem. Res., 95:

Biogasoline from Palm Oil by Simultaneous Cracking and Hydrogenation Reaction over Nimo/zeolite Catalyst

World Applied Sciences Journal 5 (Special Issue for Environment): 74-79, 2009 ISSN 1818-4952 IDOSI Publications, 2009 Biogasoline from Palm Oil by Simultaneous Cracking and Hydrogenation Reaction over