To enhance the properties of bio-based polyesters,enabling them to more closely mimic the characteristics of terephthalate-based materials,a series of aliphatic-aromatic copolyesters(P_(1)–P_(4))were synthesized via ...To enhance the properties of bio-based polyesters,enabling them to more closely mimic the characteristics of terephthalate-based materials,a series of aliphatic-aromatic copolyesters(P_(1)–P_(4))were synthesized via melt polycondensation.Diester monomers M and N were synthesized via the Williamson reaction,using lignin-derived 2-methoxyhydroquinone,methyl 4-chloromethylbenzoate,and methyl chloroacetate as starting materials.Hydroquinone bis(2-hydroxyethyl)ether(HQEE)and 1,4-cyclohexanedimethanol(CHDM)were employed as cyclic segments,while 1,4-butanediol(BDO)and 1,6-hexanediol(HDO)served as alkyl segments within the copolymer structures.The novel copolyesters exhibited molecular weights(Mw)in the range of 5.25×10^(4)–5.87×10^(4) g/mol,with polydispersity indices spanning from 2.50–2.66.Evaluation of the structural and thermomechanical properties indicated that the inclusion of alkyl segments induced a reduction in both crystallinity and molecular weight,while significantly improving the flexibility,whereas cyclic segments enhanced the processability of the copolyesters.Copolyesters P_(1) and P_(2),due to the presence of rigid segments(HQEE and CHDM),displayed relatively high glass transition temperatures(Tg>80℃)and melting temperatures(Tm>170℃).Notably,P_(2),incorporating CHDM,exhibited superior elongation properties(272%),attributed to the enhanced chain mobility resulting from its trans-conformation,while P_(1) was found to be likely brittle owing to excessive chain stiffness.Biodegradability assessment using earthworms as bioindicators revealed that the copolyesters demonstrated moderate degradation profiles,with P_(2) exhibiting a degradation rate of 4.82%,followed by P_(4) at 4.07%,P_(3) at 3.65%,and P_(1) at 3.17%.The higher degradation rate of P_(2) was attributed to its relatively larger d-spacing and lower toxicity,which facilitated enzymatic hydrolytic attack by microorganisms.These findings highlight the significance of optimizing the structural chain segments within aliphatic-aromatic copolyesters.By doing so,it is possible to significantly enhance their properties and performance,offering viable bio-based alternatives to petroleum-based polyesters such as polyethylene terephthalate(PET).展开更多
Bioplastics were first introduced as environmentally friendly materials,with properties similar to those of conventional plastics.A bioplastic is defined as biodegradable if it can be decomposed into carbon dioxide un...Bioplastics were first introduced as environmentally friendly materials,with properties similar to those of conventional plastics.A bioplastic is defined as biodegradable if it can be decomposed into carbon dioxide under aerobic degradation,or methane and CO_(2)under anaerobic conditions,inorganic compounds,and new cellular biomass,by the action of naturally occurring microorganisms.This definition however does not provide any information on the environmental conditions,timescale and extent at which decomposition processes should occur.With regard to the aquatic environment,recognized standards have been established to assess the ability of plastics to undergo biodegradation;however,these standards fail to provide clear targets to be met to allow labelling of a bioplastic as biodegradable.Moreover,these standards grant the user an extensive leeway in the choice of process parameters.For these reasons,the comparison of results deriving from different studies is challenging.The authors analysed and discussed the degree of biodegradability of a series of biodegradable bioplastics in aquatic environments(both fresh and salt water)using the results obtained in the laboratory and from on-site testing in the context of different research studies.Biochemical Oxygen Demand(BOD),CO_(2)evolution,surface erosion and weight loss were the main parameters used by researchers to describe the percentage of biodegradation.The results showed a large variability both in weight loss and BOD,even when evaluating the same type of bioplastics.This confirms the need for a reference range of values to be established with regard to parameters applied in defining the biodegradability of bioplastics.展开更多
In this study,Mg-based composites,by the addition of ZnO,Ca_(2)ZnSi_(2)O_(7),Ca_(2)MgSi_(2)O_(7),and CaSiO_(3)as bioactive agents,were fabricated using friction stir processing.The microstructure and in vitro assessme...In this study,Mg-based composites,by the addition of ZnO,Ca_(2)ZnSi_(2)O_(7),Ca_(2)MgSi_(2)O_(7),and CaSiO_(3)as bioactive agents,were fabricated using friction stir processing.The microstructure and in vitro assessment of bioactivity,biodegradation rate,and corrosion behavior of the resultant composites were investigated in simulated body fluid(SBF).The results showed that during the immersion of composites in SBF for 28 d,due to the release of Ca^(2+)and PO_(4)^(3-)ions,hydroxyapatite(HA)crystals with cauliflower shaped morphology were deposited on the surface of composites,confirming good bioactivity of composites.In addition,due to the uniform distribution of bioceramic powders throughout Mg matrix,grain refinement of the Mg matrix,and uniform redistribution of secondary phase particles,the polarization resistance increased,and the biodegradation rate of composites significantly reduced compared to monolithic Mg matrix.The polarization corrosion resistance of Mg-ZnO increased from 0.216 to 2.499 kΩ/cm^(2)compared to monolithic Mg alloy.Additionally,Mg-ZnO composite with the weight loss of 0.0217 g after 28 d immersion showed lower weight loss compared to other samples with increasing immersion time.Moreover,Mg-ZnO composite with the biodegradation rate of 37.71 mm/a exhibited lower biodegradation rate compared to other samples with increasing immersion time.展开更多
Background: Cosmetic formulations, and particularly solar products which contain mineral and chemical UV-filters, are often suspected of causing harmful effects on marine fauna and flora. After the publication of our ...Background: Cosmetic formulations, and particularly solar products which contain mineral and chemical UV-filters, are often suspected of causing harmful effects on marine fauna and flora. After the publication of our work in 2019 concerning the ecotoxicological effects of such formulations on corals (Seriatopora hystrix), we here provide some new information about the biodegradability and the ecotoxicological effects of these products on marine zoo- and phytoplankton. Therefore, we choose to realize in silico and in vitro studies of the biodegradability of several solar products but also to evaluate the ecotoxicological effects of these products on one phytoplankton, i.e. Phaeodactylum tricornutum, and one zooplankton, i.e. Acartia tonsa, of a great importance for sea species survival (notably as sources of food). Materials and methods: Two different approaches were used to study the biodegradability of the tested products: One in silico method and an in vitro one. 2 solar products were involved in the in silico study which consisted in the determination of the degradation factor (DF) of each ingredient of the tested formulas in order to finally obtain their estimated biodegradability percentage. Already available data concerning each ingredient coupled to a computer model developed with one of our partners were used to achieve this study. The in vitro study involved 8 formulas containing UV-filters and was led by following the OECD 301 F guidelines. Ecotoxicological studies of 7 of the formulas containing UV-filters were for their part realized by following the ISO 10253 guidelines for the experiments led with Phaeodactylum tricornutum, and the ISO 14669 guidelines for the experiments led with Acartia tonsa. In these studies, the effect of each tested product on crustaceans’ mortality and algal growth inhibition was assessed. Results: The in silico study predicted that formulas containing chemical UV-filters display a high biodegradability (superior to the threshold value of 60% given by the OECD 301 F guidelines). In the in vitro part of our work, the 8 tested formulas showed a biodegradability slightly inferior to the one predicted in the in silico experiments. Therefore, in order to evaluate if these calculated biodegradability value could have significant harmful effects on zoo- or phytoplankton, we studied the effect of our products regarding the growth inhibition on Phaeodactylum tricornutum and the mortality on Acartia tonsa. In this last part of the study, all the tested products were classified as “non ecotoxic” following an internal classification based on Part 4 entitled “Environmental Hazards” of Globally Harmonized System of Classification and Labelling of Chemicals (GHS), 9<sup>th</sup> edition (2021). Conclusions: These results are notably in line with those published by our teams in 2019 on the effects of solar cosmetic products on corals and seem to confirm that formulas containing mineral and chemical UV-filters can be daily used without displaying significant noxious effects on marine fauna and flora. .展开更多
聚羟基脂肪酸酯(PHA)具有良好的生物降解性、生物相容性和可持续性,在包装、食品和医疗等领域具有广泛的应用前景。因此,亟待对国内外近二十余年来的有关PHA的研究进行总结和梳理,为PHA领域的协同发展提供理论依据。本研究以Web of Scie...聚羟基脂肪酸酯(PHA)具有良好的生物降解性、生物相容性和可持续性,在包装、食品和医疗等领域具有广泛的应用前景。因此,亟待对国内外近二十余年来的有关PHA的研究进行总结和梳理,为PHA领域的协同发展提供理论依据。本研究以Web of Science(WOS)核心合集数据库和中国知网(CNKI)全文数据库为数据检索源,借助CiteSpace和VOSviewer文献计量工具,对2000-2023年PHA领域的相关文献进行知识图谱的可视化分析。结果表明,在2000-2023年间,国内外对PHA领域的研究目前处于快速增长阶段,且英文文献的发文量和年增长率均显著高于中文文献。国际对该领域的关注度和研究要早于国内,并且我国在PHA领域的研究对全球贡献较大,但有影响力的研究较为缺乏,亟待进一步提高。关键词聚类和时空突现分析表明,未来的研究热点主要集中在以下3个方面:1)降低PHA生产成本以实现工业化生产;2)关注PHA降解酶的筛选与鉴定,以及PHA降解过程中的微生物群落结构和功能研究;3)PHA的共聚改性、复合改性以及与其他生物材料的功能化改性。展开更多
基金financially supported by State Administration of Foreign Experts Affairs(SAFEA)through the High-End Foreign Expert Program(No.BG2021227001)postdoctoral funding from Wuhan University of Science and Technology(No.105008701)。
文摘To enhance the properties of bio-based polyesters,enabling them to more closely mimic the characteristics of terephthalate-based materials,a series of aliphatic-aromatic copolyesters(P_(1)–P_(4))were synthesized via melt polycondensation.Diester monomers M and N were synthesized via the Williamson reaction,using lignin-derived 2-methoxyhydroquinone,methyl 4-chloromethylbenzoate,and methyl chloroacetate as starting materials.Hydroquinone bis(2-hydroxyethyl)ether(HQEE)and 1,4-cyclohexanedimethanol(CHDM)were employed as cyclic segments,while 1,4-butanediol(BDO)and 1,6-hexanediol(HDO)served as alkyl segments within the copolymer structures.The novel copolyesters exhibited molecular weights(Mw)in the range of 5.25×10^(4)–5.87×10^(4) g/mol,with polydispersity indices spanning from 2.50–2.66.Evaluation of the structural and thermomechanical properties indicated that the inclusion of alkyl segments induced a reduction in both crystallinity and molecular weight,while significantly improving the flexibility,whereas cyclic segments enhanced the processability of the copolyesters.Copolyesters P_(1) and P_(2),due to the presence of rigid segments(HQEE and CHDM),displayed relatively high glass transition temperatures(Tg>80℃)and melting temperatures(Tm>170℃).Notably,P_(2),incorporating CHDM,exhibited superior elongation properties(272%),attributed to the enhanced chain mobility resulting from its trans-conformation,while P_(1) was found to be likely brittle owing to excessive chain stiffness.Biodegradability assessment using earthworms as bioindicators revealed that the copolyesters demonstrated moderate degradation profiles,with P_(2) exhibiting a degradation rate of 4.82%,followed by P_(4) at 4.07%,P_(3) at 3.65%,and P_(1) at 3.17%.The higher degradation rate of P_(2) was attributed to its relatively larger d-spacing and lower toxicity,which facilitated enzymatic hydrolytic attack by microorganisms.These findings highlight the significance of optimizing the structural chain segments within aliphatic-aromatic copolyesters.By doing so,it is possible to significantly enhance their properties and performance,offering viable bio-based alternatives to petroleum-based polyesters such as polyethylene terephthalate(PET).
文摘Bioplastics were first introduced as environmentally friendly materials,with properties similar to those of conventional plastics.A bioplastic is defined as biodegradable if it can be decomposed into carbon dioxide under aerobic degradation,or methane and CO_(2)under anaerobic conditions,inorganic compounds,and new cellular biomass,by the action of naturally occurring microorganisms.This definition however does not provide any information on the environmental conditions,timescale and extent at which decomposition processes should occur.With regard to the aquatic environment,recognized standards have been established to assess the ability of plastics to undergo biodegradation;however,these standards fail to provide clear targets to be met to allow labelling of a bioplastic as biodegradable.Moreover,these standards grant the user an extensive leeway in the choice of process parameters.For these reasons,the comparison of results deriving from different studies is challenging.The authors analysed and discussed the degree of biodegradability of a series of biodegradable bioplastics in aquatic environments(both fresh and salt water)using the results obtained in the laboratory and from on-site testing in the context of different research studies.Biochemical Oxygen Demand(BOD),CO_(2)evolution,surface erosion and weight loss were the main parameters used by researchers to describe the percentage of biodegradation.The results showed a large variability both in weight loss and BOD,even when evaluating the same type of bioplastics.This confirms the need for a reference range of values to be established with regard to parameters applied in defining the biodegradability of bioplastics.
文摘In this study,Mg-based composites,by the addition of ZnO,Ca_(2)ZnSi_(2)O_(7),Ca_(2)MgSi_(2)O_(7),and CaSiO_(3)as bioactive agents,were fabricated using friction stir processing.The microstructure and in vitro assessment of bioactivity,biodegradation rate,and corrosion behavior of the resultant composites were investigated in simulated body fluid(SBF).The results showed that during the immersion of composites in SBF for 28 d,due to the release of Ca^(2+)and PO_(4)^(3-)ions,hydroxyapatite(HA)crystals with cauliflower shaped morphology were deposited on the surface of composites,confirming good bioactivity of composites.In addition,due to the uniform distribution of bioceramic powders throughout Mg matrix,grain refinement of the Mg matrix,and uniform redistribution of secondary phase particles,the polarization resistance increased,and the biodegradation rate of composites significantly reduced compared to monolithic Mg matrix.The polarization corrosion resistance of Mg-ZnO increased from 0.216 to 2.499 kΩ/cm^(2)compared to monolithic Mg alloy.Additionally,Mg-ZnO composite with the weight loss of 0.0217 g after 28 d immersion showed lower weight loss compared to other samples with increasing immersion time.Moreover,Mg-ZnO composite with the biodegradation rate of 37.71 mm/a exhibited lower biodegradation rate compared to other samples with increasing immersion time.
文摘Background: Cosmetic formulations, and particularly solar products which contain mineral and chemical UV-filters, are often suspected of causing harmful effects on marine fauna and flora. After the publication of our work in 2019 concerning the ecotoxicological effects of such formulations on corals (Seriatopora hystrix), we here provide some new information about the biodegradability and the ecotoxicological effects of these products on marine zoo- and phytoplankton. Therefore, we choose to realize in silico and in vitro studies of the biodegradability of several solar products but also to evaluate the ecotoxicological effects of these products on one phytoplankton, i.e. Phaeodactylum tricornutum, and one zooplankton, i.e. Acartia tonsa, of a great importance for sea species survival (notably as sources of food). Materials and methods: Two different approaches were used to study the biodegradability of the tested products: One in silico method and an in vitro one. 2 solar products were involved in the in silico study which consisted in the determination of the degradation factor (DF) of each ingredient of the tested formulas in order to finally obtain their estimated biodegradability percentage. Already available data concerning each ingredient coupled to a computer model developed with one of our partners were used to achieve this study. The in vitro study involved 8 formulas containing UV-filters and was led by following the OECD 301 F guidelines. Ecotoxicological studies of 7 of the formulas containing UV-filters were for their part realized by following the ISO 10253 guidelines for the experiments led with Phaeodactylum tricornutum, and the ISO 14669 guidelines for the experiments led with Acartia tonsa. In these studies, the effect of each tested product on crustaceans’ mortality and algal growth inhibition was assessed. Results: The in silico study predicted that formulas containing chemical UV-filters display a high biodegradability (superior to the threshold value of 60% given by the OECD 301 F guidelines). In the in vitro part of our work, the 8 tested formulas showed a biodegradability slightly inferior to the one predicted in the in silico experiments. Therefore, in order to evaluate if these calculated biodegradability value could have significant harmful effects on zoo- or phytoplankton, we studied the effect of our products regarding the growth inhibition on Phaeodactylum tricornutum and the mortality on Acartia tonsa. In this last part of the study, all the tested products were classified as “non ecotoxic” following an internal classification based on Part 4 entitled “Environmental Hazards” of Globally Harmonized System of Classification and Labelling of Chemicals (GHS), 9<sup>th</sup> edition (2021). Conclusions: These results are notably in line with those published by our teams in 2019 on the effects of solar cosmetic products on corals and seem to confirm that formulas containing mineral and chemical UV-filters can be daily used without displaying significant noxious effects on marine fauna and flora. .
文摘聚羟基脂肪酸酯(PHA)具有良好的生物降解性、生物相容性和可持续性,在包装、食品和医疗等领域具有广泛的应用前景。因此,亟待对国内外近二十余年来的有关PHA的研究进行总结和梳理,为PHA领域的协同发展提供理论依据。本研究以Web of Science(WOS)核心合集数据库和中国知网(CNKI)全文数据库为数据检索源,借助CiteSpace和VOSviewer文献计量工具,对2000-2023年PHA领域的相关文献进行知识图谱的可视化分析。结果表明,在2000-2023年间,国内外对PHA领域的研究目前处于快速增长阶段,且英文文献的发文量和年增长率均显著高于中文文献。国际对该领域的关注度和研究要早于国内,并且我国在PHA领域的研究对全球贡献较大,但有影响力的研究较为缺乏,亟待进一步提高。关键词聚类和时空突现分析表明,未来的研究热点主要集中在以下3个方面:1)降低PHA生产成本以实现工业化生产;2)关注PHA降解酶的筛选与鉴定,以及PHA降解过程中的微生物群落结构和功能研究;3)PHA的共聚改性、复合改性以及与其他生物材料的功能化改性。
