{"title":"Biodegradability of oxidized films of polyhydroxyalkanoate copolymers containing 2-hydroxy-4-methylthiobutyrate unit in seawater","authors":"Zihan Qie, Kazuho Kosuge, Tetsuo Sakurai, Sivashankari M Ramamoorthi, Yuki Miyahara, Takeharu Tsuge","doi":"10.1016/j.polymdegradstab.2024.110975","DOIUrl":null,"url":null,"abstract":"<div><p>Polyhydroxyalkanoate (PHA) copolymers consisting of 3-hydroxybutyrate, 2-hydroxy-4-methylthiobutyrate (2H4MTB), and 2-hydroxy-4-methylvalerate were biosynthesized by recombinant <em>Escherichia coli</em> using L-methionine as the 2H4MTB precursor. The 2H4MTB unit contains a sulfide group in its side chain that can be oxidized to sulfoxide and sulfone groups by oxidants, thereby increasing the hydrophilicity of the polymer. The PHAs were biosynthesized at 3.9, 9.2, and 13.9 mol% 2H4MTB, and their polymer films were oxidized with hydrogen peroxide. The surface of the oxidized film was characterized using Fourier-transform infrared spectroscopy, Raman spectroscopy, and contact angle analysis. The oxidized films with 13.9 mol% 2H4MTB showed a 30° lower water contact angle than the non-oxidized films. To assess their marine biodegradability, the PHA films were immersed for 114 days in seawater continuously pumped from two depths (24 and 397 m) in Suruga Bay, Shizuoka, Japan. The weight loss of the films immersed in deep seawater was higher than that of those immersed in surface seawater. Additionally, there was a tendency for higher degradation of the oxidized films than that of the non-oxidized films, which was also confirmed by the biochemical oxygen demand test. In the surface morphology analysis by scanning electron microscopy, irregularities were observed in the degraded films, but their morphologies differed between the oxidized and non-oxidized films. Based on these observations, the biodegradation of the PHA films in seawater is discussed.</p></div>","PeriodicalId":406,"journal":{"name":"Polymer Degradation and Stability","volume":"229 ","pages":"Article 110975"},"PeriodicalIF":6.3000,"publicationDate":"2024-08-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Polymer Degradation and Stability","FirstCategoryId":"92","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S0141391024003197","RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"POLYMER SCIENCE","Score":null,"Total":0}
引用次数: 0
Abstract
Polyhydroxyalkanoate (PHA) copolymers consisting of 3-hydroxybutyrate, 2-hydroxy-4-methylthiobutyrate (2H4MTB), and 2-hydroxy-4-methylvalerate were biosynthesized by recombinant Escherichia coli using L-methionine as the 2H4MTB precursor. The 2H4MTB unit contains a sulfide group in its side chain that can be oxidized to sulfoxide and sulfone groups by oxidants, thereby increasing the hydrophilicity of the polymer. The PHAs were biosynthesized at 3.9, 9.2, and 13.9 mol% 2H4MTB, and their polymer films were oxidized with hydrogen peroxide. The surface of the oxidized film was characterized using Fourier-transform infrared spectroscopy, Raman spectroscopy, and contact angle analysis. The oxidized films with 13.9 mol% 2H4MTB showed a 30° lower water contact angle than the non-oxidized films. To assess their marine biodegradability, the PHA films were immersed for 114 days in seawater continuously pumped from two depths (24 and 397 m) in Suruga Bay, Shizuoka, Japan. The weight loss of the films immersed in deep seawater was higher than that of those immersed in surface seawater. Additionally, there was a tendency for higher degradation of the oxidized films than that of the non-oxidized films, which was also confirmed by the biochemical oxygen demand test. In the surface morphology analysis by scanning electron microscopy, irregularities were observed in the degraded films, but their morphologies differed between the oxidized and non-oxidized films. Based on these observations, the biodegradation of the PHA films in seawater is discussed.
期刊介绍：
Polymer Degradation and Stability deals with the degradation reactions and their control which are a major preoccupation of practitioners of the many and diverse aspects of modern polymer technology.
Deteriorative reactions occur during processing, when polymers are subjected to heat, oxygen and mechanical stress, and during the useful life of the materials when oxygen and sunlight are the most important degradative agencies. In more specialised applications, degradation may be induced by high energy radiation, ozone, atmospheric pollutants, mechanical stress, biological action, hydrolysis and many other influences. The mechanisms of these reactions and stabilisation processes must be understood if the technology and application of polymers are to continue to advance. The reporting of investigations of this kind is therefore a major function of this journal.
However there are also new developments in polymer technology in which degradation processes find positive applications. For example, photodegradable plastics are now available, the recycling of polymeric products will become increasingly important, degradation and combustion studies are involved in the definition of the fire hazards which are associated with polymeric materials and the microelectronics industry is vitally dependent upon polymer degradation in the manufacture of its circuitry. Polymer properties may also be improved by processes like curing and grafting, the chemistry of which can be closely related to that which causes physical deterioration in other circumstances.
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