聚乙烯地膜降解过程与机理研究进展
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摘要
为探讨聚乙烯地膜的降解过程及影响因素,从聚乙烯材料的分子结构与特性入手,结合国内外最新研究进展,系统论述了聚乙烯分子的降解过程、产物、机理与作用因素。文章指出聚乙烯分子较高的结晶度与相对分子质量、较强的疏水性与分子间作用力是导致其难以降解的主要因素;其中,聚乙烯分子间共价键的氧化断裂是整个降解过程的限速反应。环境中较强的光能、热能、机械作用力等能够促进聚乙烯分子键的氧化断裂,使聚乙烯分子非结晶区及小型结晶区域解聚成亲水性低聚物或小分子,并最终在微生物作用下完全分解为CO_2、H_2O、CH_4、生物质等微生物代谢产物。深入系统开展聚乙烯分子降解机理的系统研究,不仅可以科学评价残留地膜对环境的影响,而且能够指导聚乙烯地膜配方改进,降低聚乙烯地膜残留污染。
To provide insight on the degradation process of polyethylene mulch films, the progress of the most recent studies were widely reviewed, and a systematic analysis was conducted on the degradation pathway, product, mechanism, and influencing factors of polyethylenemulch films based on its molecular structure and physicochemical properties. It was noted that the high crystallinity, molecular weight, hy?drophobicity, and strong intermolecular bond made polyethylene hard to degrade naturally; molecular oxidation was the initial and rate-limit?ing step in the chain scission and degradation pathway. Many studies showed that high ultraviolet radiation, heat, and mechanical forcescould accelerate the oxidative degradation of polyethylene molecular bond, causing depolymerization of non-crystalline and small crystallineparts to hydrophilic monomers or oligomers, which would break down further to CO_2, H_2 O, CH_4, biomass, or other microbiotic metabolitesthrough microorganism bioassimilation. Thorough examination of the pathways and mechanisms that are involved in polyethylene degrada?tion could provide support for the scientific evaluation of the potential environmental hazards that are caused by mulch film residuals and potentially limit mulch film residue pollution by modifying the formulation of mulch film.
To provide insight on the degradation process of polyethylene mulch films, the progress of the most recent studies were widely reviewed, and a systematic analysis was conducted on the degradation pathway, product, mechanism, and influencing factors of polyethylenemulch films based on its molecular structure and physicochemical properties. It was noted that the high crystallinity, molecular weight, hy?drophobicity, and strong intermolecular bond made polyethylene hard to degrade naturally; molecular oxidation was the initial and rate-limit?ing step in the chain scission and degradation pathway. Many studies showed that high ultraviolet radiation, heat, and mechanical forcescould accelerate the oxidative degradation of polyethylene molecular bond, causing depolymerization of non-crystalline and small crystallineparts to hydrophilic monomers or oligomers, which would break down further to CO_2, H_2 O, CH_4, biomass, or other microbiotic metabolitesthrough microorganism bioassimilation. Thorough examination of the pathways and mechanisms that are involved in polyethylene degrada?tion could provide support for the scientific evaluation of the potential environmental hazards that are caused by mulch film residuals and potentially limit mulch film residue pollution by modifying the formulation of mulch film.
引文
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[2]严昌荣,刘恩科,舒帆,等.我国地膜覆盖和残留污染特点与防控技术[J].农业资源与环境学报,2014,31(2):95-102.YAN Chang-rong,LIU En-ke,XU Fan,et al.Review of agricultural plastic mulching and its residual pollution and prevention measures in China[J].Journal of Agricultural Resources and Environment,2014,31(2):95-102.
[3]严昌荣,何文清,刘爽,等.中国地膜覆盖及残留污染防控[M].北京:科学出版社,2015:279.YAN Chang-rong,HE Wen-qing,LIU Shuang,et al.Application of mulch films and prevention of its residual pollution in China[M].Beijing:China Science Publication,2015:279.
[4]胡国文,周智敏,张凯,等.高分子化学与物理学教程[M].北京:科学出版社,2014.HU Guo-wen,ZHOU Zhi-min,ZHANG Kai,et al.Polymer chemistry and physics[M].Beijing:Science Press,2014.
[5]Kasirajan S,Ngouajio M.Polyethylene and biodegradable mulches for agricultural applications:A review[J].Agronomy for Sustainable Development,2012,32(2):501-529.
[6]Liu E K,He W Q,Yan C R.‘White revolution’to‘white pollution’:Agricultural plastic film mulch in China[J].Environmental Research Letters,2014,9:091001.
[7]Steinmetz Z,Wollmann C,Schaefer M,et al.Plastic mulching in agriculture:Trading short-term agronomic benefits for long-term soil degradation?[J].Science of the Total Environment,2016,550:690-705.
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[13]Briassoulis D,Babou E,Hiskakis M,et al.Degradation in soil behavior of artificially aged polyethylene films with pro-oxidants[J].Journal of Applied Polymer Science,2015,132(30):42289.
[14]Wilkes R A,Aristilde L.Degradation and metabolism of synthetic plastics and associated products by Pseudomonas sp.:Capabilities and challenges[J].Journal of Applied Microbiology,2017,123(3):582-593.
[15]夏勇,黄昌猛,吕海霞,等.聚乙烯的结构、性能与应用[J].橡塑技术与装备(塑料),2017,43:42-45.XIA Yong,HUANG Chang-meng,LüHai-xia,et al.Structure,properties and applications of polyethylene[J].China Rubber/Plastics Technology and Equipment(Plastics),2017,43:42-45.
[16]潘祖仁.高分子化学[M].北京:化学工业出版社,2015.PAN Zu-ren.Polymer chemistry[M].Beijing:Chemical Industry Press,2015.
[17]欧阳平凯,姜岷,李振江,等.生物基高分子材料[M].北京:化学工业出版社,2012.OUYANG Ping-kai,JIANG Min,LI Zhen-jiang,et al.Biobased polymeric materials[M].Beijing:Chemical Industry Press,2012.
[18]Gewert B,Plassmann M M,Macleod M.Pathways for degradation of plastic polymers floating in the marine environment[J].Environmental Science:Processes&Impacts,2015,17(9):1513-1521.
[19]Krueger M C,Harms H,Schlosser D.Prospects for microbiological solutions to environmental pollution with plastics[J].Applied Microbiology and Biotechnology,2015,99(21):8857-8874.
[20]Laycock B,Nikoli?M,Colwell J M,et al.Lifetime prediction of biodegradable polymers[J].Progress in Polymer Science,2017,71:144-189.
[21]陈松哲,于九皋.LDPE/有机金属降解剂/配合剂体系降解性的研究[J].高分子材料科学与工程,2001,17(5):140-143.CHEN Song-zhe,YU Jiu-gao.A study on a novel LDPE degradable system under simulating compost condition[J].Polymer Materials Science and Engineering,2001,17(5):140-143.
[22]Albertsson A C,Karlsson S.The three stages in degradation of polymers-polyethylene as a model substance[J].Journal of Applied Polymer Science,1988,35(5):1289-1302.
[23]Ohtake Y,Ashabe H,Murakami N,et al.Biodegradation of lowdensity polyethylene,polystyrene,polyvinyl-chloride,and urea-formaldehyde resin buried under soil for over 32 years[J].Journal of Applied Polymer Science,1995,56:1789-1796.
[24]Ohtake Y,Kobayashi T,Asabe H,et al.Studies on biodegradation of LDPE:Observation of LDPE films scattered in agricultural fields or in garden soil[J].Polymer Degradation and Stability,1998,60(1):79-84.
[25]Ohtake Y,Kobayashi T,Asabe H,et al.Oxidative degradation and molecular weight change of LDPE buried under bioactive soil for 32~37 years[J].Journal of Applied Polymer Science,1996,70:1643-1659.
[26]于红军,赵英.农用塑料制品与加工[M].北京:科学技术文献出版社,2002.YU Hong-jun,ZHAO Ying.Agricultural plastic products and processing[M].Beijing:Scientific and Technical Documents Publishing House,2002.
[27]代军,晏华,郭骏骏,等.结晶度对聚乙烯热氧老化特性的影响[J].材料研究学报,2017,31(1):41-48.DAI Jun,YAN Hua,GUO Jun-jun,et al.Effects of crystallinity on degradation properties of polyethylene by thermo-oxidation aging[J].Chinese Journal of Materials Research,2017,31(1):41-48.
[28]Vasile C.Handbook of polyolefins[M].Second edition.New York:CRC Press,2000.
[29]Balasubramanian V,Natarajan K,Hemambika B,et al.High-density polyethylene(HDPE)-degrading potential bacteria from marine ecosystem of Gulf of Mannar,India[J].Letter in Applied Microbiology,2010,51:205-211.
[30]Fontanella S,Bonhomme S,Koutny M,et al.Comparison of the biodegradability of various polyethylene films containing pro-oxidant additives[J].Polymer Degradation and Stability,2010,95(6):1011-1021.
[31]代军,晏华,郭骏骏,等.密度对聚乙烯光氧老化特性的影响研究[J].高分子通报,2017(2):46-55.DAI Jun,YAN Hua,GUO Jun-jun,et al.Influence of density on degradation properties of polyethylene after photo-oxidation aging[J].Polymer Bulletin,2017(2):46-55.
[32]Roy P K,Hakkarainen M,Varma I K,et al.Degradable polyethylene:Fantasy or reality[J].Environmental Science&Technology,2011,45(10):4217-4227.
[33]Jakubowicz I.Evaluation of degradability of biodegradable polyethylene(PE)[J].Polymer Degradation and Stability,2003,80(1):39-43.
[34]Chiellini E,Corti A,D′antone S,et al.Oxo-biodegradable carbon backbone polymers:Oxidative degradation of polyethylene under accelerated test conditions[J].Polymer Degradation and Stability,2006,91(11):2739-2747.
[35]Albertsson A C,Hakkarainen M.Designed to degrade[J].Science,2017,358(6365):872-873.
[36]Hayes D G,Wadsworth L C,Sintim H Y,et al.Effect of diverse weathering conditions on the physicochemical properties of biodegradable plastic mulches[J].Polymer Testing,2017,62:454-467.
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