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完整後設資料紀錄
DC 欄位 | 值 | 語言 |
---|---|---|
dc.contributor.advisor | 吳嘉文(Chia-Wen Wu) | |
dc.contributor.author | Rusdy Zulfan | en |
dc.contributor.author | 鄭偉安 | zh_TW |
dc.date.accessioned | 2021-05-14T17:43:27Z | - |
dc.date.available | 2016-02-15 | |
dc.date.available | 2021-05-14T17:43:27Z | - |
dc.date.copyright | 2016-02-15 | |
dc.date.issued | 2015 | |
dc.date.submitted | 2015-12-04 | |
dc.identifier.citation | References
[1] Haghighi Mood, S.; Hossein Golfeshan, A.; Tabatabaei, M.; Salehi Jouzani, G.; Najafi, G. H.; Gholami, M.; Ardjmand, M., Lignocellulosic biomass to bioethanol, a comprehensive review with a focus on pretreatment. Renewable and Sustainable Energy Reviews 2013, 27, 77-93. [2]http://www.helsinki.fi/polymeerikemia/research/cellulose1.html. [3] Chen, W.; Zhong, L.-x.; Peng, X.-w.; Wang, K.; Chen, Z.-f.; Sun, R.-c., Xylan-type hemicellulose supported palladium nanoparticles: a highly efficient and reusable catalyst for the carbon-carbon coupling reactions. Catalysis Science & Technology 2014, 4 (5), 1426-1435. [4] http://www.lignoworks.ca/content/what-lignin. [5] Bozell, J. J.; Petersen, G. R., Technology development for the production of biobased products from biorefinery carbohydrates-the US Department of Energy's 'Top 10' revisited. Green Chemistry 2010, 12 (4), 539-554. [6] Toor, S. S.; Rosendahl, L.; Rudolf, A., Hydrothermal liquefaction of biomass: A review of subcritical water technologies. Energy 2011, 36 (5), 2328-2342. [7] http://www.dalinyebo.com/furfural-market. [8] Zeitsch., K. J., The chemistry and technology of furfural and its many byproducts. Amsterdam, 2000. [9] H.E. Hoydonckx, W. M. V. R., W. Van Rhijn, D.E. De Vos, P.A. Jacobs, Furfural and derivatives. Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim 2007. [10] Scholz, D.; Aellig, C.; Hermans, I., Catalytic Transfer Hydrogenation/Hydrogenolysis for Reductive Upgrading of Furfural and 5- (Hydroxymethyl)furfural. ChemSusChem 2014, 7 (1), 268. [11] Lange, J.-P.; van der Heide, E.; van Buijtenen, J.; Price, R., Furfural—A Promising Platform for Lignocellulosic Biofuels. ChemSusChem 2012, 5 (1), 151. [12] Brack, P.; Dann, S. E.; Wijayantha, K. G. U., Heterogeneous and homogenous catalysts for hydrogen generation by hydrolysis of aqueous sodium borohydride (NaBH4) solutions. Energy Science & Engineering 2015, 3 (3), 174-188. [13] Samuel, S., Catalytic production of furfuryl alcohol and catalyst therefor. Google Patents: 1956. [14] Perez, R. F.; Fraga, M. A., Hemicellulose-derived chemicals: one-step production of furfuryl alcohol from xylose. Green Chemistry 2014, 16 (8), 3942-3950. [15] Yan, K.; Wu, G.; Lafleur, T.; Jarvis, C., Production, properties and catalytic hydrogenation of furfural to fuel additives and value-added chemicals. Renewable and Sustainable Energy Reviews 2014, 38, 663-676. [16] http://www.novamolecular.com/media/THFA%20DS_R1,p. [17] Merat, N.; Godawa, C.; Gaset, A., High selective production of tetrahydrofurfuryl alcohol: Catalytic hydrogenation of furfural and furfuryl alcohol. Journal of Chemical Technology & Biotechnology 1990, 48 (2), 145-159. [18] Strassberger, Z.; Mooijman, M.; Ruijter, E.; Alberts, A. H.; Maldonado, A. G.; Orru, R. V. A.; Rothenberg, G., Finding Furfural Hydrogenation Catalysts via Predictive Modelling. Advanced Synthesis & Catalysis 2010, 352 (13), 2201-2210. [19] Gowda, A. S.; Parkin, S.; Ladipo, F. T., Hydrogenation and hydrogenolysis of furfural and furfuryl alcohol catalyzed by ruthenium(II) bis(diimine) complexes. Applied Organometallic Chemistry 2012, 26 (2), 86-93. [20] Vetere, V.; Merlo, A. B.; Ruggera, J. F.; Casella, M. L., Transition metal-based bimetallic catalysts for the chemoselective hydrogenation of furfuraldehyde. Journal of the Brazilian Chemical Society 2010, 21, 914-920. [21] Chen, X.; Sun, W.; Xiao, N.; Yan, Y.; Liu, S., Experimental study for liquid phase selective hydrogenation of furfuryl alcohol to tetrahydrofurfuryl alcohol on supported Ni catalysts. Chemical Engineering Journal 2007, 126 (1), 5 11. [22] Khan, F.-A.; Vallat, A.; Süss-Fink, G., Highly selective low-temperature hydrogenation of furfuryl alcohol to tetrahydrofurfuryl alcohol catalysed by hectoritesupported ruthenium nanoparticles. Catalysis Communications 2011, 12 (15), 1428-1431. [23] Yakabe, S.; Hirano, M.; Morimoto, T., Hydrogenation of alkenes with sodium borohydride and moist alumina catalyzed by nickel chloride. Tetrahedron Letters 2000, 41 (35), 6795 6798. [24] Fountoulaki, S.; Daikopoulou, V.; Gkizis, P. L.; Tamiolakis, I.; Armatas, G. S.; Lykakis, I. N., Mechanistic Studies of the Reduction of Nitroarenes by NaBH4 or Hydrosilanes Catalyzed by Supported Gold Nanoparticles. ACS Catalysis 2014, 4 (10), 3504-3511. [25] MacNair, A. J.; Tran, M.-M.; Nelson, J. E.; Sloan, G. U.; Ironmonger, A.; Thomas, S. P., Iron-catalysed, general and operationally simple formal hydrogenation using Fe(OTf)3 and NaBH4. Organic & Biomolecular Chemistry 2014, 12 (28), 5082-5088. [26] Sharma, P. K.; Kumar, S.; Kumar, P.; Nielsen, P., Selective reduction of mono- and disubstituted olefins by NaBH4 and catalytic RuCl3. Tetrahedron Letters 2007, 48 (49), 8704-8708. [27] http://www.seallabs.com/how-sem-eds-works.html. [28] http://www.seallabs.com/how-xps-works.html. [29]https://www2.warwick.ac.uk/fac/sci/physics/current/postgraduate/regs/mpags/ex5/techniques/structural/tem/. [30] Sing, K., The use of nitrogen adsorption for the characterisation of porous materials. Colloids and Surfaces A: Physicochemical and Engineering Aspects 2001, 187–188, 3-9. [31]http://teaching.shu.ac.uk/hwb/chemistry/tutorials/chrom/gaschrm.htm. [32] Kim, T.; Assary, R. S.; Marshall, C. L.; Gosztola, D. J.; Curtiss, L. A.; Stair, P. C., Acid-Catalyzed Furfuryl Alcohol Polymerization: Characterizations of Molecular Structure and Thermodynamic Properties. ChemCatChem 2011, 3 (9), 1451-1458. | |
dc.identifier.uri | http://tdr.lib.ntu.edu.tw/jspui/handle/123456789/4564 | - |
dc.description.abstract | 現今能源與環境議題日益漸增,在許多場合都被頻繁討論,人類毫無節制地使用石化燃料,不僅影響環境生態,更是漸漸將現代社會推向危險邊緣。而由纖維素轉換得到的生質能被科學家宣稱是解決這個問題的良藥,可作為未來替代石化燃料的綠色能源。
我們需要發展更進一步的程序得到木質纖維素的衍生物,氫化反應就是其中之一。經由糠醇 (furfuryl alcohol ,FFA)進行氫化反應可以得到的四氫糠醇 (Tetrahydrofurfuryl alcohol , THFA),被認為是農業上的「綠色溶劑」,也是可作為其他有用的化學物質之前驅物。此氫化反應通常要在高壓且100 °C以上的條件下進行,本研究則是利用硼氫化鈉作為氫氣來源,在液相且溫和的條件下 (室溫, 1 atm) 即可反應。我們已也在氣相進行反應,並且將最適條件下的結果與液相比較。銠金屬(rhodium, Rh) 附載於碳材上的商業觸媒可作為氫氣的載體,促進本氫化反應的進行。 在硼氫化鈉作為氫氣來源的系統下,此反應可在2小時內糠醇 (FFA)轉化率達到100%,並四氫糠醇 (THFA)的產率達到79% 。利用氫氣氣體進行氫化反應則可以於50 °C的條件下,在11小時糠醇(FFA)轉化率達到 94%,四氫糠醇 (THFA)的產率則是達到93%。在液相反應的選擇性相對雖然比較差,在常溫下進行反應仍是優勢,另外儀器設置簡易可以降低工業生產的成本,使此程序更具價值。或許可以成為往後進行其他的氫化反應的另一種選擇。 | zh_TW |
dc.description.abstract | Nowadays, energy and environmental issues become more intense and prevalent to be
discussed in most occasions. Uncontrolled utility of fossil fuel without any awareness to environmental impacts, certainly endangers our modern civilization. Lignocellulosicderived biomass is claimed by scientists as green-based-energy alternative to replace the fossil fuel soon or later. Further processes need to be performed to make chemicals-derived-lignocellulosic ready to be utilized, and hydrogenation is one of them. Tetrahydrofurfuryl alcohol (THFA) is one of hydrogenation’s products originated from furfuryl alcohol (FFA) which has been regarded as ―green‖ solvent in agriculture sector and precursor for another useful chemicals. Hydrogenation usually is performed under high pressure (above 10 bar) and above 100°C. Author initiated to carry on liquid-phase hydrogenation under open system and 30˚C using NaBH4 as hydrogen-generator. Gasphase hydrogenation had also been performed under certain condition, and its optimum results were used to compare to previous optimum results. Commercial catalyst rhodium embedded on carbon was chosen to carry hydrogenation. System using NaBH4 could achieve 100% conversion of FFA and 79% yield towards THFA at 30˚C for 2 hours reaction. System using H2 gas could convert 94% of FFA and 93% yield towards THFA at 50°C for 11 hours reaction. Despite of selectivity factor, NaBH4 system still achieved high yield, and not forget to mention room temperature reaction, and simple apparatus preparation became value-added. Hydrogenation using NaBH4 could become one option to be considered. | en |
dc.description.provenance | Made available in DSpace on 2021-05-14T17:43:27Z (GMT). No. of bitstreams: 1 ntu-104-R02524100-1.pdf: 1266671 bytes, checksum: 7437fca392e6b18a8bee8c118f2f3759 (MD5) Previous issue date: 2015 | en |
dc.description.tableofcontents | 1. Introduction ................................................................................................................1
1.1. Cellulose .............................................................................................................3 1.2. Hemicelluloses....................................................................................................3 1.3. Lignin..................................................................................................................4 1.4 Furfural ...............................................................................................................5 1.5 Hydrogenation.....................................................................................................6 1.6 Hydrogen storage / Hydrogen-generating agent.................................................7 1.6.1. Hydrogen-generator in complex metal........................................................7 1.6.2. Hydrogen-generator in chemical hydrides ..................................................7 1.7. Furfuryl Alcohol (FFA) ......................................................................................8 2. Paper Survey ..............................................................................................................9 2.1. Tetrahydrofurfuryl alcohol (THFA) ...................................................................9 2.2 Sodium borohydride (NaBH4) as hydrogen-generator .....................................11 2.3 Hydrogenation using NaBH4 as hydrogen-generator .......................................13 3. Objective ..................................................................................................................14 4. Experimental ............................................................................................................15 4.1 Chemicals and materials...................................................................................15 4.2 Equipments .......................................................................................................15 4.3 Hydrogenation of furfuryl alcohol....................................................................16 4.3.1 Hydrogenation using sodium borohydride (NaBH4).................................16 II 4.3.2 Hydrogenation using H2 gas......................................................................16 4.4 Characterization of material..............................................................................16 4.4.1 Principles of SEM-EDS.............................................................................17 4.4.2 Principles of XPS.......................................................................................18 4.4.3 Principles of TEM .....................................................................................18 4.4.4 N2 adsorption-desorption isotherm (BET method)....................................19 4.5 Gas chromatography .........................................................................................20 4.6 Characterization of products.............................................................................22 5. Results and Discussions...........................................................................................23 6. Conclusions..............................................................................................................36 7. Future Prospects.......................................................................................................37 References .......................................................................................................................38 Supporting Informations..................................................................................................42 | |
dc.language.iso | en | |
dc.title | 溫合條件下液相氫化應用於糠醇轉化至四氫糠醇 | zh_TW |
dc.title | Liquid-phase Hydrogenation of Furfuryl Alcohol to Tetrahydrofurfuryl Alcohol under Mild Conditions | en |
dc.type | Thesis | |
dc.date.schoolyear | 104-1 | |
dc.description.degree | 碩士 | |
dc.contributor.oralexamcommittee | 陳文華(Wen Hua Chen),鍾博文(Po-Wen Chung),陳郁文(Yu-Wen Chen) | |
dc.subject.keyword | 糠醇,四氫糠醇,氫化,硼?化?,?气, | zh_TW |
dc.subject.keyword | FFA,THFA,hydrogenation,NaBH4,H2, | en |
dc.relation.page | 44 | |
dc.rights.note | 同意授權(全球公開) | |
dc.date.accepted | 2015-12-04 | |
dc.contributor.author-college | 工學院 | zh_TW |
dc.contributor.author-dept | 化學工程學研究所 | zh_TW |
顯示於系所單位: | 化學工程學系 |
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