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
To convert the non biodegradable sodium lignin sulfonate into biodegradable substances, the sodium lignin sulfonate in the water was ozonized and the pH value, dissolved organic carbon(DOC), ultraviolet absorbency at...To convert the non biodegradable sodium lignin sulfonate into biodegradable substances, the sodium lignin sulfonate in the water was ozonized and the pH value, dissolved organic carbon(DOC), ultraviolet absorbency at λ =254 nm(UVA) and the biodegradability of the ozonation effluent were measured. The non biodegradable sodium lignin sulfonate can be partly converted into biodegradable substances by ozonation (about 38 76%). In the ozonation process, there is little DOC decrease, but much UVA decrease and obvious pH drop.展开更多
Pretreatment of Low-Density Polyethylene(LDPE)with physicochemical methods before biodegradation has been demonstrated as an effective strategy.The pretreatment of LDPE exhibited alterations in molecular structure,red...Pretreatment of Low-Density Polyethylene(LDPE)with physicochemical methods before biodegradation has been demonstrated as an effective strategy.The pretreatment of LDPE exhibited alterations in molecular structure,reducing hydrophobicity and decreasing tensile strength.Additionally,pretreating LDPE enhanced microbial biodegradability to improve biofilm formation and significantly reduced the physical weight of LDPE film.AS3–8 consortia exhibited a maximum weight loss of 8.0%±0.5%after 45 days of incubation.While Bacillus sp.AS3 and Sphingobacterium sp.AS8 demonstrated LDPE weight loss of 5.03%±1.6%and 1.6%±0.5%,respectively.The structure of LDPE was altered after incubation with the bacterial strains,resulting in a reduction in the intensity of functional groups,including C=O,C=C,N–H,and C–N.The carbonyl index(CI)of LDPE also decreased by 7.17%after the consortia AS3–8 degradation.Consortia AS3–8 significantly impacted the physical properties of LDPE by reducing the water contact angle(WCA),decreasing to 64.21°±3.69°,and tensile strength(TS),decreasing to 17.97±0.3 MPa.Moreover,the esterase activity was measured through 45 days of incubation.SDS-PAGE analysis of the AS3–8 consortia revealed bands at 35,48,and 70 kDa molecular weights,similar to known enzymes like laccase and esterase.Furthermore,SEM observations showed rough,cracked surfaces on pretreated LDPE,with biofilms present after incubation with the bacterial strains.GC–MS analysis revealed that AS3–8 consortia produced depolymerized chemicals,including alkanes,aldehydes,and esters.The LDPE biodegradation pathway was elucidated.This study addresses critical knowledge gaps in improving plastic degradation efficiency.展开更多
With the increasing accumulation of plastic pollutants in various environments,research on microorganisms(including bacteria,fungi,and algae)with plastic degradation capabilities has gained significant attention.Howev...With the increasing accumulation of plastic pollutants in various environments,research on microorganisms(including bacteria,fungi,and algae)with plastic degradation capabilities has gained significant attention.However,only a limited number of microbial plastic-degrading enzymes have been identified to date.This highlights that the degradation mechanisms employed by many plastic-degrading microorganisms,particularly filamentous fungi,remain insufficiently explored.In this study,we utilized a versatile fungal plasmid(pCT74)to express green fluorescent protein(GFP)in a marine-derived fungus Alternaria alternata strain FB1 with plastic degradation capabilities.Upon evaluating the degradation effect of polyester-type polyurethane(PU)film,we observed that different transformants exhibited three kinds of activities(the same,reduced,or enhanced degradation capability)compared to the FB1 wild-type strain.Further analysis of the plasmid fragment insertion sites in different transformants revealed that pCT74 integrates randomly into the genome of the host fungus.Notably,a direct correlation was found between the plasmid insertion site and the degradation capability of the corresponding transformant.Our findings not only redefine the potential applications of plasmid pCT74 in filamentous fungi but also show a novel research approach to identifying key enzymes involved in plastic degradation by fungi.展开更多
Poly (3-hydroxybutyrate-co-3-hydroxyvalerate)/Organophilic montmorillonite (PHBV/OMMT) nanocomposites were prepared and the biodegradability of the PHBV/OMMT nanocomposites was studied by a cultivation degrading metho...Poly (3-hydroxybutyrate-co-3-hydroxyvalerate)/Organophilic montmorillonite (PHBV/OMMT) nanocomposites were prepared and the biodegradability of the PHBV/OMMT nanocomposites was studied by a cultivation degrading method in soil suspension. The relationship between structure and biodegradability of PHBV/OMMT nanocomposites was investigated. The results showed that the biodegradability of PHBV/OMMT nanocomposites decreased with increasing amount of OMMT and it was related to the number of PHBV degrading microorganisms in degradation environment, the anti-microbial property of OMMT and the degree of crystallinity of the nanocomposites.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To convert the non biodegradable sodium lignin sulfonate into biodegradable substances, the sodium lignin sulfonate in the water was ozonized and the pH value, dissolved organic carbon(DOC), ultraviolet absorbency at λ =254 nm(UVA) and the biodegradability of the ozonation effluent were measured. The non biodegradable sodium lignin sulfonate can be partly converted into biodegradable substances by ozonation (about 38 76%). In the ozonation process, there is little DOC decrease, but much UVA decrease and obvious pH drop.
文摘Pretreatment of Low-Density Polyethylene(LDPE)with physicochemical methods before biodegradation has been demonstrated as an effective strategy.The pretreatment of LDPE exhibited alterations in molecular structure,reducing hydrophobicity and decreasing tensile strength.Additionally,pretreating LDPE enhanced microbial biodegradability to improve biofilm formation and significantly reduced the physical weight of LDPE film.AS3–8 consortia exhibited a maximum weight loss of 8.0%±0.5%after 45 days of incubation.While Bacillus sp.AS3 and Sphingobacterium sp.AS8 demonstrated LDPE weight loss of 5.03%±1.6%and 1.6%±0.5%,respectively.The structure of LDPE was altered after incubation with the bacterial strains,resulting in a reduction in the intensity of functional groups,including C=O,C=C,N–H,and C–N.The carbonyl index(CI)of LDPE also decreased by 7.17%after the consortia AS3–8 degradation.Consortia AS3–8 significantly impacted the physical properties of LDPE by reducing the water contact angle(WCA),decreasing to 64.21°±3.69°,and tensile strength(TS),decreasing to 17.97±0.3 MPa.Moreover,the esterase activity was measured through 45 days of incubation.SDS-PAGE analysis of the AS3–8 consortia revealed bands at 35,48,and 70 kDa molecular weights,similar to known enzymes like laccase and esterase.Furthermore,SEM observations showed rough,cracked surfaces on pretreated LDPE,with biofilms present after incubation with the bacterial strains.GC–MS analysis revealed that AS3–8 consortia produced depolymerized chemicals,including alkanes,aldehydes,and esters.The LDPE biodegradation pathway was elucidated.This study addresses critical knowledge gaps in improving plastic degradation efficiency.
基金Supported by the Science and Technology Innovation Project of Laoshan Laboratory(Nos.2022QNLM030004-3,LSKJ202203103)the NSFC Innovative Group Grant(No.42221005)+5 种基金the Key Collaborative Research Program of the Alliance of International Science Organizations(No.ANSO-CR-KP-2022-08)the Shandong Provincial Natural Science Foundation(No.ZR2021ZD28)the Major Research Plan of the National Natural Science Foundation(No.92351301)the Strategic Priority Research Program of the Chinese Academy of Sciences(No.XDA22050301)the Taishan Scholars Program(No.tstp20230637)the Qingdao Natural Science Foundation(No.23-2-1-182-zyyd-jch)。
文摘With the increasing accumulation of plastic pollutants in various environments,research on microorganisms(including bacteria,fungi,and algae)with plastic degradation capabilities has gained significant attention.However,only a limited number of microbial plastic-degrading enzymes have been identified to date.This highlights that the degradation mechanisms employed by many plastic-degrading microorganisms,particularly filamentous fungi,remain insufficiently explored.In this study,we utilized a versatile fungal plasmid(pCT74)to express green fluorescent protein(GFP)in a marine-derived fungus Alternaria alternata strain FB1 with plastic degradation capabilities.Upon evaluating the degradation effect of polyester-type polyurethane(PU)film,we observed that different transformants exhibited three kinds of activities(the same,reduced,or enhanced degradation capability)compared to the FB1 wild-type strain.Further analysis of the plasmid fragment insertion sites in different transformants revealed that pCT74 integrates randomly into the genome of the host fungus.Notably,a direct correlation was found between the plasmid insertion site and the degradation capability of the corresponding transformant.Our findings not only redefine the potential applications of plasmid pCT74 in filamentous fungi but also show a novel research approach to identifying key enzymes involved in plastic degradation by fungi.
基金The National Natural Science Foundation of China (No. 20374032) Chinese Education Ministry Foundation for N & T Joint Academy
文摘Poly (3-hydroxybutyrate-co-3-hydroxyvalerate)/Organophilic montmorillonite (PHBV/OMMT) nanocomposites were prepared and the biodegradability of the PHBV/OMMT nanocomposites was studied by a cultivation degrading method in soil suspension. The relationship between structure and biodegradability of PHBV/OMMT nanocomposites was investigated. The results showed that the biodegradability of PHBV/OMMT nanocomposites decreased with increasing amount of OMMT and it was related to the number of PHBV degrading microorganisms in degradation environment, the anti-microbial property of OMMT and the degree of crystallinity of the nanocomposites.
