超声制备甲醇乳化柴油影响因素的响应面法优化
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摘要
采用超声制备甲醇乳化柴油,通过正交实验筛选乳化剂配比;采用高速分散器预乳化和超声波装置深度乳化,考察了超声时间和功率、甲醇和乳化剂含量等因素对甲醇乳化柴油稳定性的影响;在单因素实验基础上,基于Box-Behnken实验设计,利用Design-Expert数据分析软件的响应面分析法优化了工艺条件,并建立了以甲醇乳化柴油稳定时间为响应值的数学模型.结果表明,适宜的乳化剂质量比为油酸:Span-80:OP-10:Tween-80:羧甲基纤维素钠=14:5:2:1:5,HLB值为4.48.各因素对甲醇乳化柴油稳定性的影响程度为乳化剂含量?超声功率?甲醇含量?超声时间,交互作用程度为超声时间和功率?超声功率和乳化剂含量?甲醇含量和乳化剂含量?超声时间和乳化剂含量?超声时间和甲醇含量;最优工艺条件为超声时间20 min、超声功率220 W、甲醇含量10%、乳化剂含量5%.在最优条件下进行实验,稳定时间实验值与预测值的相对偏差为2.69%,表明响应面拟合方程可用于超声制备甲醇乳化柴油稳定性的预测和最优工艺条件的确定.
Methanol emulsified diesel was prepared using ultrasonic, the mass ratio of emulsifier was optimized by orthogonal experiment. Pre-emulsified stage used high speed disperser, depth emulsification stage used ultrasound emulsification device. The effects of ultrasonic time, ultrasonic power, methanol content and emulsifier content on the stability of methanol emulsified diesel were investigated. Based on the experiment of single factor, the mathematical model of ultrasonic preparation methanol emulsified diesel was established with the Box-Behnken model of response surface methodology in Design-Expert software, and the parameters were optimized. The results showed that the appropriate emulsifier mass ratio was oleic acid:Span-80:OP-10:Tween-80:carboxymethyl cellulose sodium=14:5:2:1:5, and the HLB value was 4.48. The influence degree of the stability of methanol emulsified diesel was emulsifier content?ultrasonic power?methanol content?ultrasonic time. The interaction was ultrasonic time and power?ultrasonic power and emulsifier content?methanol content and emulsifier content?ultrasonic time and emulsifier content?ultrasonic time and methanol content. The optimized parameters were ultrasonic time 20 min, ultrasonic power 220 W, methanol content 10%, emulsifier content 5%. The relative deviation of the experimental stabilization time under the optimum conditions with the predicted value was 2.69%, the mathematical model of response surface fitting equation can be used to determine and predict optimum conditions of ultrasound production of methanol emulsified diesel.
Methanol emulsified diesel was prepared using ultrasonic, the mass ratio of emulsifier was optimized by orthogonal experiment. Pre-emulsified stage used high speed disperser, depth emulsification stage used ultrasound emulsification device. The effects of ultrasonic time, ultrasonic power, methanol content and emulsifier content on the stability of methanol emulsified diesel were investigated. Based on the experiment of single factor, the mathematical model of ultrasonic preparation methanol emulsified diesel was established with the Box-Behnken model of response surface methodology in Design-Expert software, and the parameters were optimized. The results showed that the appropriate emulsifier mass ratio was oleic acid:Span-80:OP-10:Tween-80:carboxymethyl cellulose sodium=14:5:2:1:5, and the HLB value was 4.48. The influence degree of the stability of methanol emulsified diesel was emulsifier content?ultrasonic power?methanol content?ultrasonic time. The interaction was ultrasonic time and power?ultrasonic power and emulsifier content?methanol content and emulsifier content?ultrasonic time and emulsifier content?ultrasonic time and methanol content. The optimized parameters were ultrasonic time 20 min, ultrasonic power 220 W, methanol content 10%, emulsifier content 5%. The relative deviation of the experimental stabilization time under the optimum conditions with the predicted value was 2.69%, the mathematical model of response surface fitting equation can be used to determine and predict optimum conditions of ultrasound production of methanol emulsified diesel.
引文
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[15]朱俊仁,郑怀礼,张智,等.响应面法优化制备PAFS-CPAM复合混凝剂及其表征[J].化工学报,2012,63(12):4019-4027.Zhu J R,Zheng H L,Zhang Z,et al.Synthesis and Characterization of Composite Flocculant PAFS-CPAM by Response Surface Methodology[J].Journal of Chemical Industry and Engineering(China),2012,63(12):4019-4027.
[16]蒋绍阶,冯欣蕊,李晓恩,等.响应面法优化制备PAC-PDMDAAC杂化絮凝剂及其表征[J].化工学报,2014,65(2):731-736.Jiang S J,Feng X R,Li X E,et al.Preparation of PAC-PDMDAAC Hybrid Flocculant by Response Surface Method and Its Characterization[J].Journal of Chemical Industry and Engineering(China),2014,65(2):731-736.
[17]张娜,郭姣,季文彬,等.响应面法优化白囊耙齿菌中腺苷的超声法提取工艺[J].中国医药工业杂志,2011,42(2):100-103.Zhang N,Guo J,Ji W B,et al.Optimal Conditions of Ultrasonic-assisted Extraction of Adenosine from Irpex Lacteus Using Response Surface Method[J].Chinese Journal of Pharmaceuticals,2011,42(2):100-103.
[18]Li X D,Jia R,Li P S,et al.Response Surface Analysis for Enzymatic Decolorization of Congo Red by Manganese Peroxidase[J].J.Mol.Catal.B:Enzym.,2009,56(1):1-6.
[19]Ferreira S L,Bruns R E,Ferreira H S,et al.Box-Behnken Design:An Alternative for the Optimization of Analytical Methods[J].Anal.Chim.Acta,2007,597(2):179-186.
[20]Quanhong L,Caili F.Application of Response Surface Methodology for Extraction Optimization of Germinant Pumpkin Seeds Protein[J].Food Chem.,2005,92(4):701-706.
[21]焦纬洲,刘有智,上官民,等.甲醇乳化柴油分散特性的研究[J].燃料化学学报,2011,39(4):311-314.Jiao W Z,Liu Y Z,Shangguan M,et al.Dispersity Characteristics of Methanol Diesel Oil Emulsified Fuel[J].Journal of Fuel Chemistry and Technology,2011,39(4):311-314.
[22]张欣然,李伟光,公绪金,等.紫外/氯耦合处理饮用水中氨氮的响应面优化[J].化工学报,2014,65(3):1049-1055.Zhang X R,Li W G,Gong X J,et al.Optimization on Combined UV/Chlorine Process for Removal of Ammoniain Drinking Water[J].Journal of Chemical Industry and Engineering(China),2014,65(3):1049-1055.
[23]JoséG G,Verónica S,Ignacio T,et al.Sonochemical Treatment of Water Polluted by Chlorinated[J].Water,2010,2(1):28-74.
[24]李彦威.在线超声间接电氧化合成苯甲醛及其衍生物的过程和机理研究[D].太原:太原理工大学,2006:43-53.Li Y W.Study on Synthesis of Benzaldehyde and Its Derivatives by Indirect Electro-Oxidation with On-line Ultrasound[D].Taiyuan:Taiyuan University of Technology,2006:43-53.
[25]Tyagi V K,Lo S L,Appels L,et al.Ultrasonic Treatment of Waste Sludge:A Review on Mechanisms and Applications[J].Crit.Rev.Env.Sci.Technol.,2014,44(11):1220-1288.
[26]Tang S Y,Tan K W,Sivakumar M.Cavitation Technology?A Greener Processing Technique for the Generation of Pharmaceutical Nano-emulsions[J].Ultrason.Sonochem.,2014,21(6):2069-2083.
[27]Wang Y,Zhou L B,,Wang H W.Diesel Emission Improvements by the Use of Oxygenated DME/Diesel Blend Fuels[J].Atmos.Environ.,2006,40(13):2313-2320.
[28]Li M K,Fogler H S.Acoustic Emulsification:Part I.The Instability of Oil-Water Interface to Form the Initial Droplets[J].J.Fluid Mech.,1978,88:499-511.
[29]何学良,詹永厚,李疏松.内燃机燃料[M].北京:中国石化出版社,1999:336-338.He X L,Zhan Y H,Li S S.Internal Combustion Engine Fuel[M].Beijing:China Petrochemical Press,1999:15-18.
[30]Xiong C H,An G J,Lu C B,et al.Study on Microstructure and Combustion-Explosion Properties of Micro-emulsified Diesel with Different Cosurfactants[J].Procedia Eng.,2014,84:402-411.
[2]Burger J L,Baibourine E,Bruno T J.C-Omparison of Diesel Fuel Oxygenate Additives to the Composition-explicit Distillation Curve Method:Part 4.Alcohols,Aldehydes,Hydroxyl Ethers,and Esters of Butanoic Acid[J].Energy Fuels,2011,26(2):1114-1123.
[3]李建彤.超声柴油微乳化研究[D].南京:南京工业大学,2004:5-27.Li J T.Study on Ultrasonic Diesel Micro-emulsification[D].Nanjing:Nanjing Technological University,2004:5-27.
[4]焦纬洲.超重力强化甲醇柴油乳化燃料制备技术[M].北京:国防工业出版社,2013:4-38.Jiao W Z.Gravity Strengthening Methanol Diesel Fuel Emulsion Preparation Techniques[M].Beijing:National Defense Industry Press,2013:4-38.
[5]李文乐.甲醇汽油在国内外应用情况及分析[J].化工进展,2010,29(3):457-464.Li W L.Methanol Gasoline and Its Application Analysis[J].Chemical Industry and Engeering Progress,2010,29(3):457-464.
[6]王军,杨许召.乳化与微乳化技术[M].北京:化学工业出版社,2012:41-43.Wang J,Yang X Z.Emulsification and Micro-emulsion Technology[M].Beijing:Chemical Industry Press,2012:41-43.
[7]Cucheval A,Chow R C Y.A Study on the Emulsification of Oil by Power Ultrasound[J].Ultrason.Sonochem.,2008,15(5):916–920.
[8]Lavilla I,Cabaleiro N,Pena F,et al.Ultrasound-assisted Emulsification Micro-extraction with Simultaneous Derivatization Coupled to Fiber Optics-based Cuvetteless UV-Vis Micro-spectrophotometry for Formaldehyde Determination in Cosmetic Samples[J].Anal.Chim.Acta,2010,674(1):59-63.
[9]Jiang H,Xu S,Cai X,et al.Comparisons of Diesel Micro-emulsion Properties Using Spontaneous Emulsifying and Ultrasonic Dispersing Methods[J].Pet.Sci.Technol.,2014,32(14):1763-1770.
[10]Chávez A,Ramírez M,Medina E,et al.Advances in the Generation of a New Emulsified Fuel[J].Heat Mass Transfer,2011,47(8):1051-1063.
[11]Gaikwad S G,Pandit A B.Ultrasound Emulsification:Effect of Ultrasonic and Physicochemical Properties on Dispersed Phase Volume and Droplet Size[J].Ultrason.Sonochem.,2008,15(4):554–563.
[12]Park S H,Kim H J,Lee C S.Effects of Dimethyl Ether(DME)Spray Behavior in the Cylinder on the Combustion and Exhaust Emissions Characteristics of a High Speed Diesel Engine[J].Fuel Process.Technol.,2010,91(5):504-513.
[13]Veljkovi?V B,Avramovi?J M,Stamenkovi?O S.Biodiesel Production by Ultrasound-assisted Transesterification:State of the Art and the Perspectives[J].Renewable Sustainable Energy Rev.,2012,16(2):1193-1209.
[14]焦纬洲,刘有智,祁贵生.柴油-甲醇-乳化剂三组元乳化液的制备及其理化特性[J].石油学报(石油加工),2011,27(1):91-94.Jiao W Z,Liu Y Z,Qi G S.Physicochemical Properties of the Emulsions Made by Diesel,Methanol and Emulsifier[J].Acta Petrolei Sinica(Petroleum Processing Section),2011,27(1):91-94.
[15]朱俊仁,郑怀礼,张智,等.响应面法优化制备PAFS-CPAM复合混凝剂及其表征[J].化工学报,2012,63(12):4019-4027.Zhu J R,Zheng H L,Zhang Z,et al.Synthesis and Characterization of Composite Flocculant PAFS-CPAM by Response Surface Methodology[J].Journal of Chemical Industry and Engineering(China),2012,63(12):4019-4027.
[16]蒋绍阶,冯欣蕊,李晓恩,等.响应面法优化制备PAC-PDMDAAC杂化絮凝剂及其表征[J].化工学报,2014,65(2):731-736.Jiang S J,Feng X R,Li X E,et al.Preparation of PAC-PDMDAAC Hybrid Flocculant by Response Surface Method and Its Characterization[J].Journal of Chemical Industry and Engineering(China),2014,65(2):731-736.
[17]张娜,郭姣,季文彬,等.响应面法优化白囊耙齿菌中腺苷的超声法提取工艺[J].中国医药工业杂志,2011,42(2):100-103.Zhang N,Guo J,Ji W B,et al.Optimal Conditions of Ultrasonic-assisted Extraction of Adenosine from Irpex Lacteus Using Response Surface Method[J].Chinese Journal of Pharmaceuticals,2011,42(2):100-103.
[18]Li X D,Jia R,Li P S,et al.Response Surface Analysis for Enzymatic Decolorization of Congo Red by Manganese Peroxidase[J].J.Mol.Catal.B:Enzym.,2009,56(1):1-6.
[19]Ferreira S L,Bruns R E,Ferreira H S,et al.Box-Behnken Design:An Alternative for the Optimization of Analytical Methods[J].Anal.Chim.Acta,2007,597(2):179-186.
[20]Quanhong L,Caili F.Application of Response Surface Methodology for Extraction Optimization of Germinant Pumpkin Seeds Protein[J].Food Chem.,2005,92(4):701-706.
[21]焦纬洲,刘有智,上官民,等.甲醇乳化柴油分散特性的研究[J].燃料化学学报,2011,39(4):311-314.Jiao W Z,Liu Y Z,Shangguan M,et al.Dispersity Characteristics of Methanol Diesel Oil Emulsified Fuel[J].Journal of Fuel Chemistry and Technology,2011,39(4):311-314.
[22]张欣然,李伟光,公绪金,等.紫外/氯耦合处理饮用水中氨氮的响应面优化[J].化工学报,2014,65(3):1049-1055.Zhang X R,Li W G,Gong X J,et al.Optimization on Combined UV/Chlorine Process for Removal of Ammoniain Drinking Water[J].Journal of Chemical Industry and Engineering(China),2014,65(3):1049-1055.
[23]JoséG G,Verónica S,Ignacio T,et al.Sonochemical Treatment of Water Polluted by Chlorinated[J].Water,2010,2(1):28-74.
[24]李彦威.在线超声间接电氧化合成苯甲醛及其衍生物的过程和机理研究[D].太原:太原理工大学,2006:43-53.Li Y W.Study on Synthesis of Benzaldehyde and Its Derivatives by Indirect Electro-Oxidation with On-line Ultrasound[D].Taiyuan:Taiyuan University of Technology,2006:43-53.
[25]Tyagi V K,Lo S L,Appels L,et al.Ultrasonic Treatment of Waste Sludge:A Review on Mechanisms and Applications[J].Crit.Rev.Env.Sci.Technol.,2014,44(11):1220-1288.
[26]Tang S Y,Tan K W,Sivakumar M.Cavitation Technology?A Greener Processing Technique for the Generation of Pharmaceutical Nano-emulsions[J].Ultrason.Sonochem.,2014,21(6):2069-2083.
[27]Wang Y,Zhou L B,,Wang H W.Diesel Emission Improvements by the Use of Oxygenated DME/Diesel Blend Fuels[J].Atmos.Environ.,2006,40(13):2313-2320.
[28]Li M K,Fogler H S.Acoustic Emulsification:Part I.The Instability of Oil-Water Interface to Form the Initial Droplets[J].J.Fluid Mech.,1978,88:499-511.
[29]何学良,詹永厚,李疏松.内燃机燃料[M].北京:中国石化出版社,1999:336-338.He X L,Zhan Y H,Li S S.Internal Combustion Engine Fuel[M].Beijing:China Petrochemical Press,1999:15-18.
[30]Xiong C H,An G J,Lu C B,et al.Study on Microstructure and Combustion-Explosion Properties of Micro-emulsified Diesel with Different Cosurfactants[J].Procedia Eng.,2014,84:402-411.