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Materials 2019, 12, 350 10 of 22 Materials 2019, 12 FOR PEER REVIEW 10 expression in host cells [120]. The application of different nanocatalysts to overcome the challenges of expression in host cells [120]. The application of different nanocatalysts to overcome the challenges biobutanol production is also receiving more interest [55]. of biobutanol production is also receiving more interest [55]. 2.2. Chemical Processes for Producing Butanol from Bio-Ethanol 2.2. Chemical Processes for Producing Butanol from Bio-Ethanol TheTchleascsliacssaicpapprporaocahchtotopprroducingbbuutatannoloflrofrmombiob-eioth-eatnhoalnporolcpeerdosceinedtshriene sttherpese. Fsitrespt,st.heFirst, the commerrcciaiallpprordoudcutcist tihsotrhoourgohulygdhelyhyderahtyedrtaotoebdtation aob1t0a0i%n anh1y0d0%rouasnshtayted.rIotuisthsteanteo.xidItiziesdthen with acetone in the presence of aluminum isopropanolate (Figure 3) to form acetaldehyde. Highly oxidized with acetone in the presence of aluminum isopropanolate (Figure 3) to form acetaldehyde. volatile acetaldehyde is separated by fractional distillation. In the second step, acetaldehyde is Highly volatile acetaldehyde is separated by fractional distillation. In the second step, acetaldehyde condensed in a strongly alkaline environment, yielding crotonaldehyde. In the final stage, is condensed in a strongly alkaline environment, yielding crotonaldehyde. In the final stage, crotonaldehyde is hydrogenated to butanol by treatment with isopropanol in the presence of titanium crotonaldehyde is hydrogenated to butanol by treatment with isopropanol in the presence of titanium or aluminum isopropanolate. or aluminum isopropanolate. Figure 3. Condensation of dehydrated bioethanol (100% anhydrous state) to butanol in the presence of Figure 3. Condensation of dehydrated bioethanol (100% anhydrous state) to butanol in the presence aluminum (or titanium) isopropanolate. of aluminum (or titanium) isopropanolate. This multistage transformation could be simplified substantially by using the borrowed hydrogen This multistage transformation could be simplified substantially by using the borrowed procedure, also known as the Gerber reaction [158]. This catalyzed reaction sequence has been hydrogen procedure, also known as the Gerber reaction [158]. This catalyzed reaction sequence has found to be highly efficient for the conversion of a broad range of alcohols [159–161], but not for been found to be highly efficient for the conversion of a broad range of alcohols [159–161], but not for ethanol [162]. Dehydrogenation of ethanol substrate has been found to be particularly difficult, ethanol [162]. Dehydrogenation of ethanol substrate has been found to be particularly difficult, while while the condensation of acetaldehyde is known to lead to a mixture of higher molecular products the condensation of acetaldehyde is known to lead to a mixture of higher molecular products and and polymeric materials (not shown). Nevertheless, a multistep process, including consecutive polymeric materials (not shown). Nevertheless, a multistep process, including consecutive oxidation oxidaotfiobniooetfhbainooelthafafnoordlianfgfoarcdeitnagldaecheytdaeld,etheydbea,sethceatbaalysezecdatalldyozlecdoanldeonlscaotinondeonfsactieotanldoefhaycdeetailndteohyde intocrottoonnaaldldeheyhdyedeanadndfifinanlalyllythtehehhydyrdorgoegneantiaotnioonfocfrocrtontoalndaelhdyedheydweitwhiptharptiarlltyialhlydhroygdernoagtednated intermediate products (2-buten-1-ol and/or butanal) over Sr–P hydroxyapatite catalyst, has been intermediate products (2-buten-1-ol and/or butanal) over Sr–P hydroxyapatite catalyst, has been reported as giving 1-butanol with 12% conversion and 67% selectivity [163]. reported as giving 1-butanol with 12% conversion and 67% selectivity [163]. There are several reports in the literature describing direct catalytic dimerization leading to There are several reports in the literature describing direct catalytic dimerization leading conversion of ethanol into 1-butanol [164], using stoichiometric or non-stoichiometric hydroxyapatite to conversion of ethanol into 1-butanol [164], using stoichiometric or non-stoichiometric [165–170], solid bases [170,171], some zeolites [172], coconut shell carbon [173] and supported metals hydroxyapatite [165–170], solid bases [170,171], some zeolites [172], coconut shell carbon [173] and (e.g., Ni, Co, Ru) [174–176], metallic (Cu, Fe, Co, Ni, Pd) supported systems modified by oxides, e.g. supported metals (e.g., Ni, Co, Ru) [174–176], metallic (Cu, Fe, Co, Ni, Pd) supported systems modified CeO2 [177] and supported palladium systems modified by KOH [178] as catalysts. These technologies by oxides, e.g., CeO [177] and supported palladium systems modified by KOH [178] as catalysts. involve a two-pha2se process, which is conducted in a fixed bed reactor with conversion in the range These technologies involve a two-phase process, which is conducted in a fixed bed reactor with of 10–20% and selectivity of up to 70% only in the case when absolute ethanol is used as starting convmerastieorniali.nAtnhoetrhaenrgperoomfi1s0in–g20c%ataalyntdicsperloecetisvsiutyseodffuopr tthoe7tr0a%nsofonrlmyaintiotnheofcbaisoeewthhanenolatobsboultuatneoeltihsanol isuspeedrfoarsmsetadritninlgiqumidatperhiasle.oAvenrostohleidrpcartoamlysistsiningacahtiaglhy-tpicrepssruorceesmsinuisreedacftor.tAhsectartanlyssftosrminatthieonof conversion of ethanol to butanol, Ir, Ru, Rh, Pd, Pt, Au, Ag and Ni supported on alumina were used. bioethanol to butanol is performed in liquid phase over solid catalysts in a high-pressure mini reactor. As catalysts in the conversion of ethanol to butanol, Ir, Ru, Rh, Pd, Pt, Au, Ag and Ni supported on alumina were used. Under optimized conditions, 18% ethanol conversion and 60% selectivity to butanol were obtained at 250 ◦C [179–181]. Detailed results are summarized in Table 3.PDF Image | Butanol Synthesis Routes for Biofuel Production
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