超高压处理下BHT在不同分子量聚乙烯中扩散的分子动力学模拟
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摘要
采用分子动力学模拟与实验结合的方法,对超高压处理条件下,抗氧化剂2,6-二叔丁基-4-甲基苯酚(BHT)在不同分子量聚乙烯(PE)中的扩散过程进行了模拟研究,通过分析超高压下PE的自由体积、PE分子链的活动性以及BHT的扩散轨迹,探讨了超高压下小分子物质在不同分子量聚乙烯中扩散的微观机理。结果表明,超高压下PE中BHT的扩散系数随压力、PE分子量的增加而减小,与迁移实验结果一致; PE的自由体积、PE分子链的运动能力随着压力、PE分子量的增加而减小,继而影响BHT的扩散,压力较低时,PE的聚合度越小,其自由体积、BHT的扩散系数和PE链的运动能力越容易受到高压的影响;超高压下BHT的运动轨迹表明,BHT在PE的基体中做缓慢蠕动式扩散,压力越高,PE分子量越大,其活动范围越小。
Combining the method of molecular dynamics simulation and experiment,under the treatment condition of high pressure,the diffusion process of antioxidant 2,6-ditert-butyl-4-methylphenol( BHT) in polyethylene( PE) with various molecular weight was simulated and investigated. The diffusion mechanism of BHT inside PE with various molecular weight under HPP was illustrated by analyzing the fractional free volume of PE,the mobility of PE chains and the movement trajectory of BHT molecules. The results indicate that the diffusion coefficient of BHT decreases with the increase of pressure and molecular weight of PE. These results are consistent with the migration experimental data. Subsequently,the free volume of PE and the mobility of PE chains could decrease with the increase of pressure and molecular weight of PE,therefore the diffusion of BHT is limited.When the pressure is low,as the decrease of the degree of polymerization,the free volume,the diffusion coefficient of BHT and PE chains could be greatly affected by high pressure. Finally,the movement trajectory of BHT in PE under HPP shows that BHT diffuses slowly in the matrix of PE,and the molecular weight of PE could increase with the increasing of pressure. Then the range of activity for BHT could be smaller.
Combining the method of molecular dynamics simulation and experiment,under the treatment condition of high pressure,the diffusion process of antioxidant 2,6-ditert-butyl-4-methylphenol( BHT) in polyethylene( PE) with various molecular weight was simulated and investigated. The diffusion mechanism of BHT inside PE with various molecular weight under HPP was illustrated by analyzing the fractional free volume of PE,the mobility of PE chains and the movement trajectory of BHT molecules. The results indicate that the diffusion coefficient of BHT decreases with the increase of pressure and molecular weight of PE. These results are consistent with the migration experimental data. Subsequently,the free volume of PE and the mobility of PE chains could decrease with the increase of pressure and molecular weight of PE,therefore the diffusion of BHT is limited.When the pressure is low,as the decrease of the degree of polymerization,the free volume,the diffusion coefficient of BHT and PE chains could be greatly affected by high pressure. Finally,the movement trajectory of BHT in PE under HPP shows that BHT diffuses slowly in the matrix of PE,and the molecular weight of PE could increase with the increasing of pressure. Then the range of activity for BHT could be smaller.
引文
[1]BIEDERMANN-BREM S,WKASPRICK N,SIMAT T,et al.Migration of polyolefin oligomeric saturated hydrocarbons(POSH)into food[J].Food Addit Contam Part A Chem Anal Control Exposure Risk Assess,2012,29(3):449-460.
[2]郭莉,郝帅,刘善晶.白酒塑料包装中增塑剂的迁移行为[J].塑料工业,2017,45(12):93-95.
[3]BALASUBRAMANIAM V,MARTINEZ-MONTEAGUDO S I,GUPTA R.Principles and application of high pressure-based technologies in the food industry[J].Annu Rev Food Sci Technol,2015,6(1):435-462.
[4]HUANG H W,WU S J,LU J K,et al.Current status and future trends of high-pressure processing in food industry[J].Food control,2017,72:1-8.
[5]JULIANO P,WKOUTCHMA T,SUI Q,et al.Polymericbased food packaging for high-pressure processing[J].Food Eng Rev,2010,2(4):274-297.
[6]唐亚丽,赵伟,卢立新.超高压作用下的食品包装问题[J].食品研究与开发,2011,32(12):193-196.
[7]GALOTTO M J,ULLOA P,ESCOBAR R,et al.Effect of high-pressure food processing on the mass transfer properties of selected packaging materials[J].Packag Technol Sci,2010,23(5):253-266.
[8]GALOTTO M J,ULLOA P A,GUARDA A,et al.Effect of high-pressure food processing on the physical properties of synthetic and biopolymer films[J].J Food Sci,2009,74(6):E304-311.
[9]SCHAUWECKER A,BALASUBRAMANIAM V M,SADLER G,et al.Influence of high-pressure processing on selected polymeric materials and on the migration of a pressure-transmitting fluid[J].Packag Technol Sci,2002,15(5):255-262.
[10]YOO S,SIGUA G,MIN D,et al.The influence of high‐pressure processing on the migration of irganox 1076 from polyethylene films[J].Packag Technol Sci,2014,27(4):255-263.
[11]CANER C,HARTE B.Effect of high-pressure processing on the migration of antioxidant Irganox 1076 from polypropylene film into a food simulant[J].J Sci Food Agric,2005,85(1):39-46.
[12]LAMBERT Y,DEMAZEAU G,LARGETEAU A,et al.Packaging for high-pressure treatments in the food industry[J].Packag Technol Sci,2000,13(2):63-71.
[13]LAMBERT Y,DEMAZEAU G,LARGETEAU A,et al.New packaging solutions for high pressure treatments of food[J].Int J High Pressure Res,2000,19(1-6):207-212.
[14]WANG Z W,LI B,LIN Q B,et al.Two-phase molecular dynamics model to simulate the migration of additives from polypropylene material to food[J].Int J Heat Mass Transfer,2018,122:694-706.
[15]陈文淑.HPVC/NBR共混物力学性能的分子模拟的研究[J].塑料工业,2013,41(6):71-77.
[16]史迎春,胡长鹰,刘芳,等.分子动力学模拟在塑料材料中迁移研究现状[J].包装工程,2015,36(11):30-35.
[17]LU W Q,LU L X,TANG Y L,et al.Impact of high-pressure processing on diffusion in polyethylene based on molecular dynamics simulation[J].Mol Simul,2017,43(7):548-557.
[18]GESTOSO P,MEUNIER M.Barrier properties of small gas molecules in amorphous cis-1,4-polybutadiene estimated by simulation[J].Mol Simul,2008,34(10-15):1135-1141.
[19]BRANDRUP J,IMMERGUT E H,GRULKE E A.Polymer handbook(4th Edition)[M].New York:Wiley,1999.
[20]王平利,王志伟,胡长鹰,等.无定形PET中小分子扩散系数的分子动力学模拟[J].化工学报,2009,60(8):1920-1925.
[21]GEORGE S C,THOMAS S.Transport phenomena through polymeric systems[J].Prog Polym Sci,2001,26(6):985-1017.
[22]SHARMA J,TEWARI K,ARYA R K.Diffusion in polymeric systems-a review on free volume theory[J].Prog Org Coat,2017,111:83-92.
[23]RAMESH N,DAVIS P K,ZIELINSKI J M,et al.Application of free-volume theory to self diffusion of solvents in polymers below the glass transition temperature:A review[J].J Polym Sci,Part B:Polym Phys,2011,49(23):1629-1644.
[24]WARFIELD R W.Compressibility of bulk polymers[J].Polym Eng Sci,1966,6(2):176-180.
[25]FRALDI M,CUTOLO A,ESPOSITO L,et al.Delamination onset and design criteria of multilayer flexible packaging under high pressure treatments[J].Innovative Food Sci Emerging Technol,2014,23:39-53.
[26]SANSONE L,ALDI A,MUSTO P,et al.Assessing the suitability of polylactic acid flexible films for high pressure pasteurization and sterilization of packaged foodstuff[J].JFood Eng,2012,111(1):34-45.
[27]BARTELS C R,CRIST B,GRAESSLEY W W.Self-diffusion coefficient in melts of linear polymers:Chain length and temperature dependence for hydrogenated polybutadiene[J].Macromolecules,1984,17(12):2702-2708.
[28]PEARSON D,VER STRATE G,VON MEERWALL E,et al.Viscosity and self-diffusion coefficient of linear polyethylene[J].Macromolecules,1987,20(5):1133-1141.
[29]SHEPHERD J E,MCDOWELL D L,JACOB K I.Modeling morphology evolution and mechanical behavior during thermo-mechanical processing of semi-crystalline polymers[J].J Mech Phys Solids,2006,54(3):467-489.
[30]CLARKE J H R,BROWN D.Molecular dynamics computer simulation of chain molecule liquids[J].Mol Phys,1986,58(4):815-825.
[2]郭莉,郝帅,刘善晶.白酒塑料包装中增塑剂的迁移行为[J].塑料工业,2017,45(12):93-95.
[3]BALASUBRAMANIAM V,MARTINEZ-MONTEAGUDO S I,GUPTA R.Principles and application of high pressure-based technologies in the food industry[J].Annu Rev Food Sci Technol,2015,6(1):435-462.
[4]HUANG H W,WU S J,LU J K,et al.Current status and future trends of high-pressure processing in food industry[J].Food control,2017,72:1-8.
[5]JULIANO P,WKOUTCHMA T,SUI Q,et al.Polymericbased food packaging for high-pressure processing[J].Food Eng Rev,2010,2(4):274-297.
[6]唐亚丽,赵伟,卢立新.超高压作用下的食品包装问题[J].食品研究与开发,2011,32(12):193-196.
[7]GALOTTO M J,ULLOA P,ESCOBAR R,et al.Effect of high-pressure food processing on the mass transfer properties of selected packaging materials[J].Packag Technol Sci,2010,23(5):253-266.
[8]GALOTTO M J,ULLOA P A,GUARDA A,et al.Effect of high-pressure food processing on the physical properties of synthetic and biopolymer films[J].J Food Sci,2009,74(6):E304-311.
[9]SCHAUWECKER A,BALASUBRAMANIAM V M,SADLER G,et al.Influence of high-pressure processing on selected polymeric materials and on the migration of a pressure-transmitting fluid[J].Packag Technol Sci,2002,15(5):255-262.
[10]YOO S,SIGUA G,MIN D,et al.The influence of high‐pressure processing on the migration of irganox 1076 from polyethylene films[J].Packag Technol Sci,2014,27(4):255-263.
[11]CANER C,HARTE B.Effect of high-pressure processing on the migration of antioxidant Irganox 1076 from polypropylene film into a food simulant[J].J Sci Food Agric,2005,85(1):39-46.
[12]LAMBERT Y,DEMAZEAU G,LARGETEAU A,et al.Packaging for high-pressure treatments in the food industry[J].Packag Technol Sci,2000,13(2):63-71.
[13]LAMBERT Y,DEMAZEAU G,LARGETEAU A,et al.New packaging solutions for high pressure treatments of food[J].Int J High Pressure Res,2000,19(1-6):207-212.
[14]WANG Z W,LI B,LIN Q B,et al.Two-phase molecular dynamics model to simulate the migration of additives from polypropylene material to food[J].Int J Heat Mass Transfer,2018,122:694-706.
[15]陈文淑.HPVC/NBR共混物力学性能的分子模拟的研究[J].塑料工业,2013,41(6):71-77.
[16]史迎春,胡长鹰,刘芳,等.分子动力学模拟在塑料材料中迁移研究现状[J].包装工程,2015,36(11):30-35.
[17]LU W Q,LU L X,TANG Y L,et al.Impact of high-pressure processing on diffusion in polyethylene based on molecular dynamics simulation[J].Mol Simul,2017,43(7):548-557.
[18]GESTOSO P,MEUNIER M.Barrier properties of small gas molecules in amorphous cis-1,4-polybutadiene estimated by simulation[J].Mol Simul,2008,34(10-15):1135-1141.
[19]BRANDRUP J,IMMERGUT E H,GRULKE E A.Polymer handbook(4th Edition)[M].New York:Wiley,1999.
[20]王平利,王志伟,胡长鹰,等.无定形PET中小分子扩散系数的分子动力学模拟[J].化工学报,2009,60(8):1920-1925.
[21]GEORGE S C,THOMAS S.Transport phenomena through polymeric systems[J].Prog Polym Sci,2001,26(6):985-1017.
[22]SHARMA J,TEWARI K,ARYA R K.Diffusion in polymeric systems-a review on free volume theory[J].Prog Org Coat,2017,111:83-92.
[23]RAMESH N,DAVIS P K,ZIELINSKI J M,et al.Application of free-volume theory to self diffusion of solvents in polymers below the glass transition temperature:A review[J].J Polym Sci,Part B:Polym Phys,2011,49(23):1629-1644.
[24]WARFIELD R W.Compressibility of bulk polymers[J].Polym Eng Sci,1966,6(2):176-180.
[25]FRALDI M,CUTOLO A,ESPOSITO L,et al.Delamination onset and design criteria of multilayer flexible packaging under high pressure treatments[J].Innovative Food Sci Emerging Technol,2014,23:39-53.
[26]SANSONE L,ALDI A,MUSTO P,et al.Assessing the suitability of polylactic acid flexible films for high pressure pasteurization and sterilization of packaged foodstuff[J].JFood Eng,2012,111(1):34-45.
[27]BARTELS C R,CRIST B,GRAESSLEY W W.Self-diffusion coefficient in melts of linear polymers:Chain length and temperature dependence for hydrogenated polybutadiene[J].Macromolecules,1984,17(12):2702-2708.
[28]PEARSON D,VER STRATE G,VON MEERWALL E,et al.Viscosity and self-diffusion coefficient of linear polyethylene[J].Macromolecules,1987,20(5):1133-1141.
[29]SHEPHERD J E,MCDOWELL D L,JACOB K I.Modeling morphology evolution and mechanical behavior during thermo-mechanical processing of semi-crystalline polymers[J].J Mech Phys Solids,2006,54(3):467-489.
[30]CLARKE J H R,BROWN D.Molecular dynamics computer simulation of chain molecule liquids[J].Mol Phys,1986,58(4):815-825.