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  An overview on the production of bio-methanol as potentialrenewable energy N.S. Shamsul a , S.K. Kamarudin a,b, n , N.A. Rahman b , N.T. Ko 󿬂 i b a Fuel Cell Institute, Universiti Kebangsaan Malaysia, 43600 UKM Bangi, Selangor, Malaysia b Department of Chemical and Process Engineering, Universiti Kebangsaan Malaysia, 43600 UKM Bangi, Selangor, Malaysia a r t i c l e i n f o  Article history: Received 4 September 2012Received in revised form6 February 2014Accepted 15 February 2014Available online 12 March 2014 Keywords: Bio-methanolBiomassWasteTechno-economy a b s t r a c t The depletion of the fossil fuel supply and the environmental pollution caused by fossil fuel combustion havebecome major worldwide problems. Biomass is a renewable resource that has the potential to replace fossilfuels. One of the valuable biomass products is bio-methanol, which can be used to generate electricity andpower for portable applications. This paper discusses the potential of bio-methanol as a renewable resourcetaking into account the world demand, economic assessment, power density and possible applications. Ittherefore presents the unique properties of bio-methanol as a potential energy resource. It also discusses thevarious types of biomass that can be obtained fromwaste products and the different processes that have beendeveloped for the production of bio-methanol fIn addition, it discusses the current problems facing bio-methanol production and the further technological improvements that are needed to support the futureenergy requirements. Overall, the yield of bio-methanol depends on the type of process used and theassociated kinetic parameters of the conversionprocess. Catalysts havebeen used inthe thermo-chemical andbio-chemical conversion of carbon dioxide into bio-methanol. Several advanced methods have been recentlyintroduced to enhance the production of methanol, but further research is required before these can be usedfor large-scale bio-methanol production. &  2014 Elsevier Ltd. All rights reserved. Contents 1. Introduction. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 5792. The potential of methanol as a future renewable energy source . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 5792.1. World demand for methanol . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 5792.2. Economy assessment of methanol . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 5792.3. Applications of methanol . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 5802.4. Power density of methanol. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 5803. The potential of using biomass and waste for bio-methanol production . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 5803.1. Types of bio-mass . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 5803.1.1. Agricultural waste . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 5823.1.2. Forestry waste . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 5823.1.3. Livestock and poultry waste . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 5823.1.4. Fishery waste. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 5823.1.5. Sewage sludge . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 5824. Bio-methanol production . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 5824.1. Pyrolysis. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 5834.2. Gasi 󿬁 cation . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 5834.3. Biosynthesis. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 5834.4. Methane. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 5844.5. Carbon dioxide and carbon monoxide . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 5844.6. Photo-electrochemical (PEC) processes. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 585 Contents lists available at ScienceDirect journal homepage: www.elsevier.com/locate/rser Renewable and Sustainable Energy Reviews http://dx.doi.org/10.1016/j.rser.2014.02.0241364-0321  &  2014 Elsevier Ltd. All rights reserved. n Corresponding author. Tel.:  + 60 389216422; fax:  + 60 389216148. E-mail address:  ctie@vlsi.eng.ukm.my (S.K. Kamarudin).Renewable and Sustainable Energy Reviews 33 (2014) 578 – 588  4.7. Electrolysis. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 5855. Kinetic parameters . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 5856. Current problems with bio-methanol production . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 5857. Conclusion . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 586Acknowledgement. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 587References . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 587 1. Introduction Technology enhancements and human development contributetothe continuous increase in the worldwide energy demand [1 – 3].There are three categories of energy sources: fossil fuels, renew-able and nuclear energy. Fossil fuels, such as coal, petroleum andnatural gas, are non-renewable energy sources that will bedepleted in the next few years [4 – 6]. The renewable energysources include solar, wind, hydroelectric, biomass and geother-mal energy, whereas nuclear energy is derived from  󿬁 ssion andfusion reactions [6]. Fossil fuel source depletion has increased theneed to reduce the consumption of fossil fuels [7 – 9]. However, thedepletion is not the only current concern with fossil fuel use. Theenvironmental degradation caused by burning fossil fuels and thewaste products produced have created an imbalance in the atmo-spheric carbon dioxide (CO 2 ) levels, which has become the majorcontributor to global warming [10]. In addition, the municipalsolid wastes from human and animal activities have also con-tributed to the environmental degradation. Therefore, it has beensuggested that this waste should be recycled or converted intoenergy [11 – 14].The disposal of agricultural, human and animal waste (solid)that is categorised as biomass material is yet another problem thatshould be addressed. In addition to its use as a plant fertiliser,animal waste can be converted via a chemical reaction and thushas the potential to be used as a chemical feedstock. The fossil fuelemission during fuel processing has prompted the search forrenewable sources that emit zero or low pollution. The use of bio-methanol from biomass is more advantageous than fossilproducts because of its low pollution emission and raw materialavailability; furthermore, the characteristics of this alcohol areidentical to those of fossil fuel. Hence, biomass is a renewableenergy source that can potentially replace fossil fuels [7,15,16]. It iswell-known in certain countries, such as Brazil and the US, thatbio-methanol from biomass can produce electrical energy [17].This paper discusses the various types of biomass that canbe obtained from waste, the different processes that are availablefor methanol production and the current problems that areinvolved in the production of methanol. In essence, this paperwill discuss the potential of bio-methanol as a renewable powerresource. 2. The potential of methanol as a future renewableenergy source  2.1. World demand for methanol In 2000, approximately 6.2 billion tons of carbon was emittedinto the atmosphere as CO 2  and approximately 40% of this wasemitted during the production of electricity. A survey from the U.S.Department of Energy revealed that the consumption of electri-city, which increases signi 󿬁 cantly every year, is projected toincrease by 44% from 2006 to 2030 [18]. By 2050, road transporta-tion is expected to be the largest contributor to greenhouseemissions. In Europe, the renewable energy target for 2010 wasapproximately 5.75% of the transport fuels sold, and this targetwill likely increase to 10% in 2020. If this trend continues, therenewable energy target for the transport fuels sold should reach27% by 2025. Compared with the gasoline and fossil dieseldemands (51% and 22%, respectively), biofuels are expected toconstitute 75% of the total demand [19].Natural gas comprises approximately 80% of the total cost of methanol production in Western European methanol plants [20].In fact, the total cost of methanol production from CO 2  is 500 – 600 €  t  1 ; however, the cost of producing methanol from biomass isapproximately 300 – 400  €  t  1 of methanol [21]. Thus, biomassprocessing is the most cost-effective of the processes that havebeen developed for the production of methanol from renewablesources [19]. The production cost of bio-methanol is lower thanthat of light oil, which is used in power stations [7]. Hasegawaet al. [17] reported that the U.S. and Brazil currently monopolisethe biomass processes for bio-ethanol production using grain orthe combination of sugar cane and corn. However, because thefeedstock (corn) for these bio-ethanol products is a food product,this practice has attracted criticism given the increasing foodprices and the global food shortage. Although both methanoland ethanol are liquid hydrocarbons, ethanol is twice as expensiveas methanol. However, the location, capacity, mode of operation,operating conditions and the purity grade of the  󿬁 nal product arefactors that affect the economics of methanol production.  2.2. Economy assessment of methanol As one of alternative compound, more than 75% of methanolproduced by natural gas, synthesis from the syngas. Today, about90 methanol plants generated with a total annual capacity of morethan 50 million tons. Fig. 1 presents the price for production of methanol from fossil resources. The price of methanol is not stablefrom year 2006 until 2009 but after that, the price is increaseduntil year 2011. Therefore, as demand for the methanol increased,it is expected that the price of methanol will also increase in nextfuture [22].Adamson et al. claimed that about 3.13 USD GJ  1 in year 1990required for production of methanol via electrolysis process withhydropower feedstock. While for gasi 󿬁 cation of biomass, plant size Fig. 1.  Methanex non-discounted reference price of methanol (MNDRP) [22]. N.S. Shamsul et al. / Renewable and Sustainable Energy Reviews 33 (2014) 578 – 588  579  1650 dry tons/day in 1991 required 9.55 – 14.10 $GJ  1 of methanolcost and with same plant size, required costing 9.83 – 14.18USD GJ  1 in year 1993 [21]. Pedersen et al. [22] who studied the production of methanol from biomass by steam reforming (SR)and partial oxidation (POX) of technical and economic assessmentin year 2012 claimed that methanol can be produced at acompetitive price of 687 USD t  1 by farm scale, 419 by largescale of partial oxidation and 453 USD t  1 by steam reforming. Itshows the highest price of production in farm scale, whilethe cheapest production price is achieved by the large scale plantvia partial oxidation. Even though it required largest annualexpenditures, the larger throughput of methanol outweighs thisdisadvantage.Kumabe et al. [7] reported that plant size is 91.1 kg dry s  1 wood and the wood procurement cost is 7.1 ¥ kg dry  1 , the BTL MeOH cost is 12.8 k¥ m  3 MeOH, while it is 78 k¥ m  3 MeOHwhen the plant size is 1.16 kg dry s  1 wood and the wood procure-ment cost is 0 ¥ kg dry  1 , by biomass to liquid process (gasi 󿬁 cation).Lundgren et al. [23] investigate the feasibility of an innovative way of producing methanol from off-gases and they proved that integratingmethanol production in a steel plant can be made economicallyfeasible and may result in environmental bene 󿬁 ts as well as energyef  󿬁 ciency improvements.  2.3. Applications of methanol As a renewable carbon resource, biomass can be convertedfrom a solid phase into a wide range of chemicals that can be usedas liquid fuels (biofuels), such as bio-oil, bio-ethanol, bio-metha-nol, bio-diesel, liquid hydrocarbons, mixed alcohols, acetic acidand formaldehyde. However, bio-methanol has the most potentialas a biofuel for power generation because it is a distributed form of energy production [24]. Moreover, methanol is suitable for addi-tional downstream applications, such as fuel cell-powered vehi-cles, because it can be easily degraded to carbon dioxide andhydrogen in the presence of steam. Methanol is the simplestorganic liquid hydrogen carrier that acts as a hydrogen storagecompound. It is also an attractive automotive fuel because of itsphysical and chemical characteristics. A mixture of methanol andconventional petrol, such as M85 (85% methanol and 15% unleadedgasoline), has enabled the production of methanol-fuelled vehicleswithout necessitating any major technical modi 󿬁 cations to theexisting vehicles. Since methanol was introduced in China in 2008,the amount of E85 used in China has included the blending of more than 1 billion US gallons (3,800,000 m 3 ) of methanol intofuel [25]. In addition to its applications as an automotive fuel andas feedstock for chemical production, methanol can be used forbiodiesel production by vegetable oil (triglyceride) transesteri 󿬁 ca-tion and as a fuel for direct methanol fuel cells without an on-boardreformer. Fuel-grade methanol is a clean and ef  󿬁 cient alternativefuel for gas turbines in power industry applications [26].As alternative fuels for motors, methanol, ethanol and DME achievea similar reduction in carbon dioxide emissions; however, if theamount of heat used in their production is taken into account, theuse of methanol and DME results in a higher CO 2  reduction thanethanol [27].In the transportation sector, methanol is superior to gasolinebecause it burns at a lower temperature. The low volatility of methanol reduces the risk of an explosion or  󿬂 ash  󿬁 re. Further-more, methanol  󿬁 res can be easily extinguished with waterbecause methanol is less  󿬂 ammable than gasoline. Methanol canalso be easily and safely transported in its liquid phase by road,rail, ocean tanker or pipeline, which makes it more advantageousthan hydrogen due to the problems associated with hydrogenstorage. In addition, methanol has lower volumetric energy con-tent than gasoline, which would require minimal changes to theexisting fuel distribution networks. Moreover, methanol has agreater octane number (1 0 7) than gasoline (98) [8,19]; thus, thisfuel is an attractive choice for high-compression engine applica-tions given its compression ratio modi 󿬁 cation, valve timing, lowcost and increased power [8]. In addition, methanol has a wider 󿬂 ammability range than petrol (6 – 36.5 vol% and 1 – 7.6 vol% formethanol and petrol, respectively); hence, even though petrolrapidly reaches its lower  󿬂 ammability limit, it also rapidly reachesits upper limit [21].The required feedstock for producing formal-dehyde, methyl tertiary butyl ether (MTBE), acetic acid, methylmethacrylate and dimethyl terephthalate includes approximately70% methanol. In addition, methanol is a well-known anti-frostagent, inhibitor and solvent [20].The rapid growth of chemical technologies and industries thatcontribute to air and environmental pollution requires somelimitations to prevent the excessive emission of carbon dioxideinto the atmosphere. A carbon dioxide recycling system that usescarbon dioxide from  󿬂 ue gas and renewable hydrogen from theelectrolysis of wind farms was developed to produce methanol.Approximately 0.19 t of bio-methanol can be produced from 1 t of fossil fuel, which could result in a decrease of 0.42 MTon in CO 2 emissions per year; a total of 0.27 t of CO 2  are emitted per ton of methanol at a power energy cost of 0.01 USD kWh  1 using anelectrolysis system [20]. Naqvi et al. [28] had presented black liquor gasi 󿬁 cation (BLG) systems for methanol production andreduction of CO 2  as potential technology candidates for the futuredeployment.  2.4. Power density of methanol Methanol exhibits more ef  󿬁 cient energy storage than com-pressed hydrogen in terms of weight and volume. Methanol has ahigher volumetric energy density (99 gL   1 ) than liquid hydrogen(71 gL   1 ) and therefore does not require the use of a cryogeniccontainer that needs to be maintained at a temperature of   253  1 C [25]. As the primary fuel in fuel cells, methanol consistsof a 6100 kW kg  1 energy density, which maximises the operationallife-time of the fuel cell in the limited fuel cartridge volume [29]. Inaddition, a fuel cell that uses methanol as the primary fuel cellachieves an energy output of 480 Wh in a volume of 0.6 L and a runtime of 19 h, which signi 󿬁 es a 7.4 WL   1 power density and a289.2 Wh kg  1 energy density. A methanol – water mixture that isused indirectly as a polymer-electrolyte membrane fuel producesenergy output of 166 Wh with 0.24 L of methanol over 7 h, whichcorresponds to a power density of 16.9 WL   1 and an energy densityof 112.2 Wh L   1 [30]. A Japanese company, Sharp Corporation,achieved a power density of 0.3 Wcc  1 in a direct methanol fuelcell (DMFC) that gave ef  󿬁 cient power generation in mobile equip-ment from a small cell volume; this power density is, to date, thehighest that has been attained [31]. Hamelinck et al. [32] conducted a technical and economic evaluation of methanol production andfound that the overall energy ef  󿬁 ciency for bio-methanol produc-tion was 55% of the high heating value. A hot gas cleaning processimproved the production system performance. An input of 400 MWproduced biofuels at US $ 8 – 12GJIt  1 . 3. The potential of using biomass and wastefor bio-methanol production  3.1. Types of bio-mass Biomass is an organic or carbonaceous material that storessunlight in the form of chemical energy through photosynthesis.It can be used as an alternative for fossil fuels for several reasons:(1) it is a source of sustainable renewable energy, (2) it is N.S. Shamsul et al. / Renewable and Sustainable Energy Reviews 33 (2014) 578 – 588 580  environmentally friendly, (3) it has signi 󿬁 cant economic potentialand (4) it creates energy security [33]. Biomass is de 󿬁 ned accord-ing to its purpose and application, which are different dependingon the  󿬁 eld. There are  󿬁 ve categories of biomass: wood fuelsderived from natural forest and woodland sources (e.g., sawdust),agricultural residues (e.g., rice husks, straw and manure), energycrops that are grown exclusively for energy production (e.g., cornand palm oil), urban waste (e.g., municipal solid waste andsewage) and refused-derived biomass fuel (e.g., wooden pellets).The classi 󿬁 cation of these biomass resources is detailed in Fig. 2.The utilisation of waste biomass is one of the alternatives toovercome the dependence on fossil fuels. Fig. 3 shows the currentstocks of worldwide waste biomass which consist of animal,agricultural, forestry and industry types of waste. Among thisbiomass, cattle manure is the highest biomass residues generated(23 EJyr  1 ) followed by industrial logs (20 EJyr  1 ) [34]. Theamounts of animal waste generated conclude that it has highpotential inuse asrenewableenergy. There are a numberofbene 󿬁 tsassociated with using these second generation biofuels, whichinclude a reduction in the amount of food supplies that wouldneed to be diverted to fuel production, a more environmentallyfriendly production with less greenhouse gas (GHG) emissions,more competitive prices and a wide choice of feedstock [35]. Themain component of biomass, cellulosic, is an important component 0 5 10 15 20 25 RiceWhea t MaizeRoots and TubersSugar cane residues (top and leaves ) BaggaseCattleSwinePoultryHorsesBuffaloesCamelsGoatsSheepIndustrial logsFuel logsWood waste Amount of biomass residues (EJ/yr) Fig. 3.  Amount of biomass residue in the world [36]. Biomass Resources Plantation (Production group) Untapped Natural ResourceAgriculture, Livestock, Forestry and Fishery group Other WasterouAgriculture: Rice husk, Rice straw, Wheat straw, Vegetable residue, etc Livestock: Animal waste, Butchery waste, Forestry: Forest residue, Thinned wood, Fishery: Processing waste, Dead fish, Industry: Sewage sludge, Organic Household:Garbae Human waste etc.Continental area: Grain, Plant, Vegetable, Fat and oil, etc. Water area: Algae, Photosynthetic Fig. 2.  Biomass resources categorisation [33]. N.S. Shamsul et al. / Renewable and Sustainable Energy Reviews 33 (2014) 578 – 588  581
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