Current Situations and Prospects of Oil/Fat Resources for Biodiesel Production

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1 Current Situations and Prospects of Oil/Fat Resources for Biodiesel Production Hiroaki Imahara 1, Eiji Minami 1, Makoto Hattori 2, Hiroshi Murakami 2, Nobuaki Matsui 2 and Shiro Saka 1,* 1 Graduate School of Energy Science, Kyoto University, Kyoto, Japan 2 Toyota Tsusho Corporation, Nagoya, Japan Abstract: Biodiesel is an alternative for fossil diesel that is produced by transesterification of oils/fats with methanol. For further dissemination, waste oils/fats should be efficiently utilized especially in Japan. In this study, therefore, estimation was made on the amount of waste oils/fats emerged annually in Japan. Concurrently, waste oils/fats were collected from several sites and subjected to the analyses such as acid value, water content, peroxide value, iodine value and fatty acid composition for evaluating as a feedstock of biodiesel. Based on these lines of information, it was found that dark oil containing a high content of fatty acids and used cooking oil remain useful for biodiesel production. A set of analyses showed that dark oil can be converted into biodiesel only with noncatalytic method such as supercritical methanol method, whereas used cooking oils can be available with alkali-catalyzed method. From these findings, it was clarified that waste oils/fats can be efficiently utilized as well as virgin ones. Keywords: Biodiesel, Waste Oils/Fats, Feedstock Availability, Acid Value, Fatty Acid Composition 1. INTRODUCTION Biodiesel fuel (BDF) is an alternative for fossil diesel that is produced by transesterification of oils/fats with alcohol. With increasing concern to the environmental issues such as global warming and air pollution, BDF use has been recognized and promoted worldwide, especially in EU and US. According to the statistics [1], production of BDF in these leading countries is estimated to reach about 2.6 million tons in For further dissemination of this environmentally-friendly fuel, feedstock availability is one of the important issues. In Japan, heavy dependence of oils/fats resources abroad has been a serious problem. In 2004, for instance, oils/fats import comprises 87 % of their total supply [2]. Taking account of this situation, it is inevitable in Japan to use waste oils/fats as primary raw material of BDF. For example, BDF production project has started in Kyoto city since Waste oils/fats are collected from households and food service industries to be used as a raw material of BDF with alkali-catalyzed method. Approximately 1,500 tons of BDF are produced annually. Utilization of these waste oils/fats is appreciated because it not only mitigates many environmental problems but also improve process economy by reducing the cost of raw material. From this point, BDF production from waste oils/fats should be promoted worldwide. Virgin oils/fats consist of triglycerides as the main component and free fatty acids as minor component. However, waste oils/fats often have undergone long-term degradation, thereby being high in free fatty acids and water content due to hydrolysis reaction. Furthermore, degree of the degradation heavily depends on when and where they are disposed of. For example, among various waste oils/fats, the main component of the dark oil is free fatty acids, whereas that of used cooking oil from households is triglycerides. As is well known for alkali-catalyzed method, free fatty acid is converted to saponified product. This sapnification causes not only decrease in methyl ester (BDF) yield, but also formation of emulsion during washing process, which makes separation of water and methyl ester difficult. Moreover, water should be removed before the reaction since it hinders the catalytic activity for both acid- and alkali-catalyzed methods. Supercritical methanol method, on the other hand, can be applied to almost any kind of waste oils/fats [3-5]. It is, however, still ongoing for development toward practical use, and conventional and commercial BDF production is carried out with alkali-catalyzed method. Therefore, it is useful to investigate the content of both free fatty acid and water in various waste oils/fats. On the other hand, BDF must satisfy specification standards in EU and US. These standards include not only ester content but also some of the fuel characteristics, such as iodine value, cold flow properties, which are attributed to fatty acid composition of oils/fats. Among them, oxidation stability is one of the important characteristics. For example, highly unsaturated oils/fats such as sunflower oil tend to be susceptible to oxidation. Since BDF takes over the characteristics of raw material, it is important to investigate degree of oxidation, which can be evaluated with peroxide value, with respect to waste oils/fats themselves. Based on these backgrounds, in this study, estimation was made on the amount of waste oils/fats emerged annually in Japan. Various characteristics were analyzed for actual waste oils/fats collected from various sites. 2. EXPERIMENTAL 2.1 Estimation on the amount of waste oils/fats in Japan In Japan, waste oils/fats were discarded from various sites: edible oils/fats refinery, oils/fats products manufacturer, food manufacturing industry, food service industry and households. Crude oils/fats are refined in an edible oils/fats refinery accompanied by disposal of dark oil. Oils/fats products manufacturer produces margarine and shortening. Food manufacturing industry produces snacks, instant food, fish cake, etc. with frying oil at several food manufacturing factories and the used frying oil is disposed of regularly. Food service industry indicates various restaurants using cooking oil. Amount of waste oils/fats discarded from the above sites were estimated based on the previous investigation, which is conducted by the Institute of Energy Economics, and the present status of oils/fats in Japan, Ministry of Agriculture, Forestry and Fishery [2,6]. In addition, the amount of dark oil was especially investigated in this study and reflected on the estimation. It should be noted that annual consumption of refined oils/fats in Japan ends up in approximately 3 million tons; 2.5 million for Corresponding author: saka@energy.kyoto-u.ac.jp This paper is an excerpt from the original paper submitted to Japan Society of Energy and Resources in June

2 edible use, 450 thousand tons for non-edible use and 50 thousand tons for export. Oils/fats for export was omitted from the estimation since they were discarded abroad. Non-edible oils, most of which is used for industrial purposes such as lubricant, were also not taken into account in the estimation since these oils were discarded in a from completely different from the original triglyceride structure. 2.2 Analytical conditions Fifty-one waste oils/fats were collected from the above sites in Japan. One of the examples of collection is shown in Fig.1, which was from one of the food service industries. Contaminants such as insoluble residues were removed by filtration. These samples were then analyzed in terms of acid value (AV), water content, iodine value (IV), peroxide value (POV) and fatty acid composition. Acid value, which is a measure of the free fatty acid content, was determined in accordance with No in the Standard Methods for the Analysis of Fats, Oils and Related Materials [7]. Water content was measured with Karl Fischer equipment with the above standard method, No Iodine value, which indicates the degree of unsaturation, was determined according to the standard method, No Peroxide value, which suggests hydroperoxide concentration, was measured in accordance with standard methods, No Fatty acid composition was determined by gas chromatography in accordance with the standard method, No Fig.1 Waste oils and fats collected 3. RESULTS AND DISCUSSION 3.1 Estimation on waste oils/fats discarded Dark oil is discarded from edible oils/fats refinery. After oils are expelled and extracted from oil seeds, remaining free fatty acids are removed by undergoing neutralization process. The obtained alkali oil sludge, which is a mixture of saponified products, lipids and other minor compounds, is acidified with strong acid such as hydrochloric acid or sulfuric acid to be dark oil (acid oil). According to the hearing investigation to several edible oils/fats refineries, total oils/fats production in Japan is approximately 1,800 thousand ton/year, accompanied by approximately 120 thousand ton/year of alkali oil sludge. When lipid in the oil sludge is also taken into account, approximately 30 thousand tons of dark oil, which accounts for nearly 1.7% of the total oils/fats production, was estimated to be discarded annually as a result of refinery. Ratio of disposal to supply in Japan is estimated as in Table 1. Waste oils from oils/fats products manufacturer is not disposed of during production process. However, Some of the products, which accounts for 5 % of its supply, come out from a market due to expiration date as waste oil. Ratios of disposal to supply for food manufacturing industry, food service industry and households are 10%, 30% and 40%, respectively. In this study, these values were used with recent statistic data about supply and demand in 2006 as shown in Table 2. It is clearly seen from Table 2 that the total amount of waste oils/fats in Japan ends up in 450~570 thousand tons; 120~240 thousand tons of which comes out from households and just thrown away as garbage. On the other hand, waste oils/fats from the other sites end up in approximately 330(= ) thousand tons; excluding 30 thousand tons of dark oil, 90% of the rest have been already utilized for feeding or industrial purpose, according to waste oil dealers estimation [6], i.e., approximately 30 thousand tons are not utilized effectively. Therefore, total amount of waste oils/fats that is not effectively utilized currently becomes approximately 180~300 thousand tons including the amount of dark oil and waste oils from households. From these lines of information, waste oils/fats produced in Japan was summarized in Fig.2. 2

3 It should be noted that when these waste oils are utilized effectively as a feedstock of BDF, they become at most 330 thousand kilo liters, which accounts for approximately 0.8% of annual fossil diesel fuel consumption of 40 million kilo liters [8]. Table 1 Ratio of disposal of waste oils/fats to their supply Disposal sites of waste oils/fats Disposal (gram/person/year) Ratio of disposal to supply (%) Ratio of products back from market to supply (%) Edible oils/fats refinery Oils/fats products manufacturer Food manufacturing industry Food service industry Households * For households, there are two different estimations conducted as in the table and these values are consistent with each other. Table 2 Supply of edible oils/fats and disposal of their wastes Disposal sites of waste oils/fats Supply of Disposal (gram/person/year)) Disposal of waste oils/fats edible oils/fats *1 Supply *2 Wastes (1,000 ton/year) (1,000 ton/year) Edible oils/fats refinery (1) (1,800 *3 ) Edible oils/fats refinery (2) (2,530 19,500 3,270~4, ~540 Oils/fats products manufacturer 430 3, Food manufacturing industry 840 6, Food service industry 660 *4 5,000 1, Households 600 *4 4, ~1, ~240 *1:Values taken from the reference 6 *2:Population in Japan is assumed to be 130 million *3:Production of vegetable oils/fats *4:Value determined by the assumption where 48% of oils/fats for direct use corresponds to households. (1,800 (Domestically produced)) Dark oil 34~ 030 Collected 300 (Processing) 1, Oils/fats products manufacturer Waste oil 34~ Edible oils/fats refinery Imported 2,530 1,260 (Direct use) Food manufacturing industry Food service industry Households Waste oil 34~ 080 Used cooking oil 34~ 200 Used cooking oil 120 ~ Waste oils 450 ~ 570 Fig.2 Waste oils/fats produced in refinery process (x 1,000 tons) Uncollected 150 ~ Characterization of various waste oils/fats Table 3 shows water content, acid value, peroxide value and iodine value for waste oils/fats collected from the above sites. It is clearly seen that all dark oils show notably high acid value in the range from 130~190, which suggests that dark oil usually contains 65~95% of free fatty acids. In addition, these dark oils were high in water content up to about 2 %. As is well known, alkalicatalyzed method is not applicable for low-quality oil/fat feedstocks that are high in free fatty acid content and water content. These results clearly indicate that dark oil can be converted to BDF with non-catalytic conversion method such as supercritical methanol method, but cannot with alkali-catalyzed method. Waste oil from food manufacturing industry is found to be low in both acid value and water content as in Table 3. It was also 3

4 observed that peroxide value is low, thereby not being deteriorated from the viewpoint of oxidation stability. Therefore, this oil seems to have a satisfactory quality for successful conversion as well as refined oils/fats. However, this oil is also quite low in iodine value. Therefore, BDF from this waste oil may be adequate in oxidation stability, but inadequate in cold flow properties. In terms of used cooking oils from food service industry and households, acid value and peroxide value of the former is relatively higher than that of the latter. This might to be attributed to the difference in frequency of use before disposal. From the results of acid value, both used cooking oils have a satisfactory quality to be converted to BDF with alkali-catalyzed method. However, it is preferable in the case of used cooking oil from food service industry to be converted with two-step conversion method that consists of acid-catalyzed method and subsequent alkali-catalyzed method. Table 3 Characterization of various waste oils/fats Waste oils/fats Water content Acid value Peroxide value Iodine value (%) mg(koh)/g meq/kg g(i 2 )/100g Dark oil A Dark oil B Dark oil C Waste oil from Food manufacturing industry Food service industry Household < A B C < A B C Fatty acid composition of various waste oils/fats Table 4 shows fatty acid composition of various waste oils/fats. It can be seen that dark oil A, which is derived from a fish oil refinery, contains highly poly-unsaturated fatty acids such as eicosapentanoic acid (C 20:5 ), docosahexaenoic acid (C 22:6 ). Since high unsaturation results in poor oxidation stability, dark oil A should be decreased in degree of unsaturation before used as a feedstock of BDF by hydrogenation, for instance. However, hydrogenation of oils causes an increase in degree of saturation, which aggravates cold flow properties. Since dark oil A is originally high in saturated fatty acid content, hydrogenation is not preferable. Therefore, waste oils derived from fish oil had better be used as a source of valuable poly-unsaturated fatty acid. Dark oil B, which is derived from rapeseed oil refinery, shows similar fatty acid composition to that of rapeseed (canola) oil and high in unsaturated fatty acid, especially oleic acid content. Therefore, BDF from dark oil B is adequate from the viewpoint of both oxidation stability and cold flow properties. Dark oil C and waste oil from food manufacturing industry, which are derived from palm oil, are high in saturated fatty acid content, namely palmitic acid (C 16:0 ). Therefore, biodiesel from these oils has a poor operability under cold temperature. In order to utilize these oils effectively, mixing with other oils/fats is one of the solutions to decrease degree of saturation. food service industry and/or households usually consist of rapeseed oil and soybean oil. Although saturated fatty acid content is relatively higher than that of refined rapeseed oil, cold flow properties is still adequate when converted to BDF. From the viewpoint of oxidation stability, addition of antioxidant is preferable due to slightly higher linoleic acid (C 18:2 ) content. In this way, characteristics of waste oils/fats are quite different from each other, and it is thus difficult to collect waste oils that have constant quality at steadily frequency. It should be noted that characteristics of feedstocks have a great effect on the quality of BDF. Therefore, survey on the characteristics of waste oils/fats is of importance and further investigation should be thus desirable. 3.4 Prospects of BDF production business As mentioned above, there are many kinds of waste oils/fats in Japan depending on the sites. For development of BDF production business, however, feedstocks must be constant in quality, quantity and price. In addition, it should be effectively collected. When these requirements are taken into account, dark oil is an appropriate candidate. Since dark oil accompanies refinery of edible oils/fats, steady supply can be expected in an edible oils/fats refinery. Moreover, price of the feedstock is expected to be low and refineries are interested in its effective use as a feedstock of BDF. Table 4 Fatty acid composition of various waste oils/fats Waste oils/fats Fatty acid composition (wt%) C 16:0 C 16:1 C 18:0 C 18:1 C 18:2 C 18:3 C 20:1 C 20:5 C 22:6 Others Dark oil A Dark oil B Dark oil C Waste oil from Food manufacturing industry

5 Food service industry Household A B C A B C Dark oil is high in free fatty acid, thus difficult to be converted to BDF with alkali-catalyzed method. Therefore, supercritical methanol method is currently regarded as the most viable technology for commercial BDF production from dark oil. In Japan, there are 49 factories producing edible oils/fats, in which 30 thousand tons of dark oil were annually disposed of. In some of the large factories, 3,500 ton/year of dark oil is able to be collected. With additional 1,500 ton/year of waste oils collected by other neighboring companies, households and waste oil dealers, large-scale plant that has 5,000 ton/year production capacity can be realized; 1,500 tons is achievable value as in the BDF production project from waste oils/fats in Kyoto City. As shown in Fig.2, annual availability of uncollected BDF is 150~270 thousand tons. If all of these waste oils were converted, almost the same amount of BDF would be produced. On the other hand, in case 5% replacement of fossil diesel fuel with BDF (B5) is assumed, 2 million kilo liters (1.8 million tons) of BDF is required. It is obvious that up to 270 thousand tons of BDF is not enough to satisfy the required amount. Under these circumstances, it is important in the future to look for feedstocks not only in Japan but also in Southeast Asian region, where a plenty of oils/fats resources are available. For example, production of palm oil from oil palm (Elaeis guineensis) has been increasing recently to be the second in production after soybean oil, which is the most largely produced vegetable oil worldwide. Plantation of oil palm is now spreading all over in Malaysia and Indonesia. In addition, seeds from physic nut (Jatropha curcas), sandbox tree (Hura crepitans) and sea mango tree (Cerbera manghas) are rich in oil content. However, due to toxic substances contained in seeds, these are inedible, thus being of high potential for BDF production. From these lines of information, it was clarified that for the promotion of BDF production in Japan, not only effective utilization of waste oils/fats discarded but also collection of oils/fats resources in Southeast Asia are getting more important. 4. ACKNOWLEDGMENTS This work has been done under the Kyoto University 21 COE program Establishment of COE on Sustainable-Energy System ( ~ ) supported by the Ministry of Education, Culture, Sports, Science and Technology, Japan, and the Highly Efficient Bioenergy Conversion Project ( ~ ) from New Energy and Industrial Technology Development Organization (NEDO), for which the authors are highly acknowledged. 5. REFERENCES [1] F.O.LICHT (2005) WORLD OF BIODIESEL 2005, World Ethanol & Biofuels Report, 3(13), pp [2] Ministry of Agriculture, Forestry and Fisheries, Japan (2005) Wagakuni no Yushi-jijo (Present Status of Oils/fats in Japan), pp (in Japanese). [3] Saka, S. and Kusdiana, D. (2001) Biodiesel fuel from rapeseed oil as prepared in supercritical methanol, Fuel, 80, pp [4] Saka, S. (2005) Biodiesel Fuel Production by Supercritical Methanol Technology, J. Jpn. Inst. Energy, 84, pp [5] Minami, E. and Saka, S. (2006) Kinetics of hydrolysis and methyl esterification for biodiesel production in two-step supercritical methanol process, Fuel, 85(17-18), pp [6] The Institute of Energy Economics, Japan (1994) Shokubutsuhaiyu no sekiyudaitai enerugi toshiteno saiseikanousei chousa (Feasibility Study on Waste Vegetable Oils/fats as Substitute for Fossil-derived Fuel), pp (in Japanese). [7] Japan Oil Chemists Society (1996) Standard Methods for Fats, Oils and Related Materials (in Japanese). [8] Ministry of Economy, Trade and Industry, Japan (2004) Energy Production and Demand Statistics monthly Report (METI), pp (in Japanese). 5

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