The integration of interfacial photothermal conversion and hydrovoltaic effect into bifunctional evaporators has emerged as a hopeful approach to address water and energy scarcities.However,developing low-cost bifunct...The integration of interfacial photothermal conversion and hydrovoltaic effect into bifunctional evaporators has emerged as a hopeful approach to address water and energy scarcities.However,developing low-cost bifunctional evaporators and elucidating the freshwater-electricity co-generation mechanism remain challenging.In this work,we prepare porous carbon from waste polyester through a metalorganic framework(MOF)-assisted carbonization strategy and subsequently fabricate a bifunctional evaporator for freshwater-hydroelectricity co-generation.The porous carbon contains rich oxygen-containing groups and shows hierarchical micro-and mesopores with a high specific surface area of 904 m^(2)g^(-1).The porous carbon-based evaporator shows broadband and high light absorption,localized thermal management,good hydrophilicity,and high flexibility.Benefiting from these merits,it achieves high-performance freshwater and hydroelectricity co-generation,with the opencircuit voltage of 250 mV,the short-circuit current of 14μA,and the evaporation rate of 2.34 kg m^(-2)h^(-1).Hence,it is ranked among the most efficient freshwater-hydroelectricity co-generator.Additionally,the weakened hydrogen-bonding network reduces water evaporation enthalpy to 1.7 kJ g^(-1).Mechanistic investigations reveal that selective Na+interaction induces differential ion migration rate to generate streaming potential,as evidenced by molecular dynamics simulations.Meanwhile,the photothermal effect enhances voltage output by promoting interfacial ion concentration gradients.During the outdoor freshwater-electricity co-generation,it shows the voltage output of 250 mV and freshwater production of 2.34 kg m-2.This work not only puts forward a new platform to fabricate advanced evaporators from low-cost waste plastics but also unravels the freshwater-electricity co-generation mechanism,offering scalable strategies to tackle freshwater and energy crises.展开更多
Copper manufactured by laser powder bed fusion(LPBF)process typically exhibits poor strength-ductility coordination,and the addition of strengthening phases is an effective way to address this issue.To explore the eff...Copper manufactured by laser powder bed fusion(LPBF)process typically exhibits poor strength-ductility coordination,and the addition of strengthening phases is an effective way to address this issue.To explore the effects of strengthening phases on Cu,Cu-carbon nanotubes(CNTs)composites were prepared using LPBF technique with Cu-CNTs mixed powder as the matrix.The formability,microstructure,mechanical properties,electrical conductivity,and thermal properties were studied.The result shows that the prepared composites have high relative density.The addition of CNTs results in inhomogeneous equiaxed grains at the edges of the molten pool and columnar grains at the center.Compared with pure copper,the overall mechanical properties of the composite are improved:tensile strength increases by 52.8%and elongation increases by 146.4%;the electrical and thermal properties are also enhanced:thermal conductivity increases by 10.8%and electrical conductivity increases by 12.7%.展开更多
Renewable 2,5-furandicarboxylic acid-based polyesters are one of the most promising materials for achieving plastic replacement in the age of energy and environmental crisis.However,their properties still cannot compe...Renewable 2,5-furandicarboxylic acid-based polyesters are one of the most promising materials for achieving plastic replacement in the age of energy and environmental crisis.However,their properties still cannot compete with those of petrochemical-based plastics,owing to insufficient molecular and/or microstructure designs.Herein,we utilize the Ti_(3)C_(2)T_(x)-based MXene nanosheets for decorating carbon nanotube(CNT)and obtaining the structurally stable and highly dispersed dendritic heterostructured MXene@CNT,that can act as multi-roles,i.e.,polycondensation catalyst,crystal nucleator,and interface enhancer of polyester.The biobased MXene@CNT/polybutylene furandicarboxylate(PBF)(denoted as MCP)nanocomposites are synthesized by the strategy of“in situ catalytic polymerization and hot-pressing”.Benefiting from the multi-scale interactions(i.e.,covalent bonds,hydrogen bonds,and physical interlocks)in hybrid structure,the MCP presents exceptional mechanical strength(≈101 MPa),stiffness(≈3.1 GPa),toughness(≈130 MJ m^(-3)),and barrier properties(e.g.,O_(2)0.0187 barrer,CO_(2)0.0264 barrer,and H2O 1.57×10^(-14) g cm cm^(-2) s Pa)that are higher than most reported bio-based materials and engineering plastics.Moreover,it also displays satisfactory multifunctionality with high reprocessability(90%strength retention after 5 recycling),UV resistance(blocking 85%UVA rays),and solvent-resistant properties.As a state-of-art high-performance and multifunctional material,the novel bio-based MCP nanocomposite offers a more sustainable alternative to petrochemical-based plastics in packaging and engineering material fields.More importantly,our catalysis-interfacial strengthening integration strategy opens a door for designing and constructing high-performance bio-based polyester materials in future.展开更多
电控离子交换技术(electrochemically switched ion exchange,ESIX)是将电活性离子交换材料(EXIMs)沉积或涂覆在导电基底上,通过电化学控制导电基底上活性材料氧化还原状态实现目标离子置入与释放,从而实现离子的分离。该技术具有痕量...电控离子交换技术(electrochemically switched ion exchange,ESIX)是将电活性离子交换材料(EXIMs)沉积或涂覆在导电基底上,通过电化学控制导电基底上活性材料氧化还原状态实现目标离子置入与释放,从而实现离子的分离。该技术具有痕量提取、无二次污染、速率可控、高选择性等优点。通过共沉淀法制备Ni Fe Mn LDH,并将其与碳纳米管(CNTs)、聚偏二氟乙烯(PVDF)混合涂覆到石墨板上,制得NiFeMn LDH/CNTs/PVDF膜电极。NiFeMn LDH层板上具有丰富的羟基官能团,可与W(Ⅵ)发生羟基配位;层间的阴离子与W(Ⅵ)进行离子交换,可为W(Ⅵ)提供丰富的活性位点。在ESIX系统中,膜电极对W(Ⅵ)的吸附容量可达122.10 mg·g^(-1),且W(Ⅵ)与Mo(Ⅵ)、Cl^(-)、■分离因子(■)分别为1.25、19.60、35.80,实现了W(Ⅵ)选择性分离。此外,该膜电极具有优异的循环稳定性,为钨的高效分离提供了新的方向。展开更多
Chemical modification of polymers represents a pivotal method for achieving functionalized polymer materials.However,due to the lack of post-functional handle,the chemical modification of polyester materials remains a...Chemical modification of polymers represents a pivotal method for achieving functionalized polymer materials.However,due to the lack of post-functional handle,the chemical modification of polyester materials remains a significant challenge.Ring-opening copolymerization of cyclic anhydride and epoxides is a powerful approach to synthesize polyesters.In this work,we for the first time demonstrate the functionalizability of polyesters synthesized with brominated anhydride monomers.The post-functionalization is amenable to a wide variety of reactive groups and reactions with high yields.With multiple well-established functionalization pathways of brominated polyester materials and optimized the conditions for the modification reactions,a series of functionalized polyester materials can be obtained with high yields,providing new insights for the research about functionalization of polymers.展开更多
The asymmetric alternating copolymerization of meso-epoxide and cyclic anhydrides provides an efficient access to enantiopure polyesters.Contrary to the extensive investigation of the stereochemistry resulting from ep...The asymmetric alternating copolymerization of meso-epoxide and cyclic anhydrides provides an efficient access to enantiopure polyesters.Contrary to the extensive investigation of the stereochemistry resulting from epoxide building block,the chirality from anhydride and the configurational match with epoxide remain elusive.Herein,we discover that the bimetallic chromium catalysts have led to an obvious enhancement in terms of reactivity and enantioselectivity for the asymmetric copolymerization of meso-epoxide with various non-symmetric chiral anhydrides.Up to 97%ee was obtained during the asymmetric copolymerization of cyclohexene oxide(CHO)with(R)-methylsuccinic anhydride(R-MSA),and three-or four-carbon chiral centers were simultaneously installed in the aliphatic polyester backbone.In particular,the different combinations of stereochemistry in epoxide and anhydride building blocks considerably affect the thermal properties and crystalline behaviors of the resulting polyesters.This study uncovers an interesting method for regulating polymer crystallinity via matching the chirality of different monomers.展开更多
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
基金supported by the National Natural Science Foundation of China(52373099)Interdisciplinary Research Program of Huazhong University of Science and Technology(5003013161)+1 种基金Innovation and Talent Recruitment Base of New Energy Chemistry and Device(B21003)Hubei Integrative Technology and Innovation Center for Advanced Fiberous Materials(XC202502)。
文摘The integration of interfacial photothermal conversion and hydrovoltaic effect into bifunctional evaporators has emerged as a hopeful approach to address water and energy scarcities.However,developing low-cost bifunctional evaporators and elucidating the freshwater-electricity co-generation mechanism remain challenging.In this work,we prepare porous carbon from waste polyester through a metalorganic framework(MOF)-assisted carbonization strategy and subsequently fabricate a bifunctional evaporator for freshwater-hydroelectricity co-generation.The porous carbon contains rich oxygen-containing groups and shows hierarchical micro-and mesopores with a high specific surface area of 904 m^(2)g^(-1).The porous carbon-based evaporator shows broadband and high light absorption,localized thermal management,good hydrophilicity,and high flexibility.Benefiting from these merits,it achieves high-performance freshwater and hydroelectricity co-generation,with the opencircuit voltage of 250 mV,the short-circuit current of 14μA,and the evaporation rate of 2.34 kg m^(-2)h^(-1).Hence,it is ranked among the most efficient freshwater-hydroelectricity co-generator.Additionally,the weakened hydrogen-bonding network reduces water evaporation enthalpy to 1.7 kJ g^(-1).Mechanistic investigations reveal that selective Na+interaction induces differential ion migration rate to generate streaming potential,as evidenced by molecular dynamics simulations.Meanwhile,the photothermal effect enhances voltage output by promoting interfacial ion concentration gradients.During the outdoor freshwater-electricity co-generation,it shows the voltage output of 250 mV and freshwater production of 2.34 kg m-2.This work not only puts forward a new platform to fabricate advanced evaporators from low-cost waste plastics but also unravels the freshwater-electricity co-generation mechanism,offering scalable strategies to tackle freshwater and energy crises.
基金National Key Research and Development Program of China(2023YFB4606400)Supported by Longmen Laboratory Frontier Exploration Topics(LMQYTSKT003)。
文摘Copper manufactured by laser powder bed fusion(LPBF)process typically exhibits poor strength-ductility coordination,and the addition of strengthening phases is an effective way to address this issue.To explore the effects of strengthening phases on Cu,Cu-carbon nanotubes(CNTs)composites were prepared using LPBF technique with Cu-CNTs mixed powder as the matrix.The formability,microstructure,mechanical properties,electrical conductivity,and thermal properties were studied.The result shows that the prepared composites have high relative density.The addition of CNTs results in inhomogeneous equiaxed grains at the edges of the molten pool and columnar grains at the center.Compared with pure copper,the overall mechanical properties of the composite are improved:tensile strength increases by 52.8%and elongation increases by 146.4%;the electrical and thermal properties are also enhanced:thermal conductivity increases by 10.8%and electrical conductivity increases by 12.7%.
基金financial supports from the National Natural Science Foundation of China(Grant No.NSFC52473104)National Key R&D Program of China(Grant No.2022YFC2104500)+3 种基金Zhejiang Provincial Natural Science Foundation of China(Grant No.Y24B040002)Ningbo 2025 Key Scientific Research Programs(Grant No.2022Z160)the China Postdoctoral Science Foundation(Grant No.2023M733601)the Ningbo Natural Science Foundation(Grant No.2023I333&2023J409).
文摘Renewable 2,5-furandicarboxylic acid-based polyesters are one of the most promising materials for achieving plastic replacement in the age of energy and environmental crisis.However,their properties still cannot compete with those of petrochemical-based plastics,owing to insufficient molecular and/or microstructure designs.Herein,we utilize the Ti_(3)C_(2)T_(x)-based MXene nanosheets for decorating carbon nanotube(CNT)and obtaining the structurally stable and highly dispersed dendritic heterostructured MXene@CNT,that can act as multi-roles,i.e.,polycondensation catalyst,crystal nucleator,and interface enhancer of polyester.The biobased MXene@CNT/polybutylene furandicarboxylate(PBF)(denoted as MCP)nanocomposites are synthesized by the strategy of“in situ catalytic polymerization and hot-pressing”.Benefiting from the multi-scale interactions(i.e.,covalent bonds,hydrogen bonds,and physical interlocks)in hybrid structure,the MCP presents exceptional mechanical strength(≈101 MPa),stiffness(≈3.1 GPa),toughness(≈130 MJ m^(-3)),and barrier properties(e.g.,O_(2)0.0187 barrer,CO_(2)0.0264 barrer,and H2O 1.57×10^(-14) g cm cm^(-2) s Pa)that are higher than most reported bio-based materials and engineering plastics.Moreover,it also displays satisfactory multifunctionality with high reprocessability(90%strength retention after 5 recycling),UV resistance(blocking 85%UVA rays),and solvent-resistant properties.As a state-of-art high-performance and multifunctional material,the novel bio-based MCP nanocomposite offers a more sustainable alternative to petrochemical-based plastics in packaging and engineering material fields.More importantly,our catalysis-interfacial strengthening integration strategy opens a door for designing and constructing high-performance bio-based polyester materials in future.
文摘电控离子交换技术(electrochemically switched ion exchange,ESIX)是将电活性离子交换材料(EXIMs)沉积或涂覆在导电基底上,通过电化学控制导电基底上活性材料氧化还原状态实现目标离子置入与释放,从而实现离子的分离。该技术具有痕量提取、无二次污染、速率可控、高选择性等优点。通过共沉淀法制备Ni Fe Mn LDH,并将其与碳纳米管(CNTs)、聚偏二氟乙烯(PVDF)混合涂覆到石墨板上,制得NiFeMn LDH/CNTs/PVDF膜电极。NiFeMn LDH层板上具有丰富的羟基官能团,可与W(Ⅵ)发生羟基配位;层间的阴离子与W(Ⅵ)进行离子交换,可为W(Ⅵ)提供丰富的活性位点。在ESIX系统中,膜电极对W(Ⅵ)的吸附容量可达122.10 mg·g^(-1),且W(Ⅵ)与Mo(Ⅵ)、Cl^(-)、■分离因子(■)分别为1.25、19.60、35.80,实现了W(Ⅵ)选择性分离。此外,该膜电极具有优异的循环稳定性,为钨的高效分离提供了新的方向。
基金financially supported by the National Key R&D Program of China(No.2021YFA1501700)the Science and Technology Development Plan of Jilin Province(Nos.20230101042JC and 20210201059GX)+1 种基金the National Natural Science Foundation of China,Basic Science Center Program(No.51988102)the National Natural Science Foundation of China(Nos.52203017 and 52073272)。
文摘Chemical modification of polymers represents a pivotal method for achieving functionalized polymer materials.However,due to the lack of post-functional handle,the chemical modification of polyester materials remains a significant challenge.Ring-opening copolymerization of cyclic anhydride and epoxides is a powerful approach to synthesize polyesters.In this work,we for the first time demonstrate the functionalizability of polyesters synthesized with brominated anhydride monomers.The post-functionalization is amenable to a wide variety of reactive groups and reactions with high yields.With multiple well-established functionalization pathways of brominated polyester materials and optimized the conditions for the modification reactions,a series of functionalized polyester materials can be obtained with high yields,providing new insights for the research about functionalization of polymers.
基金financially supported by the National Natural Science Foundation of China(Nos.22071016 and 21920102006)。
文摘The asymmetric alternating copolymerization of meso-epoxide and cyclic anhydrides provides an efficient access to enantiopure polyesters.Contrary to the extensive investigation of the stereochemistry resulting from epoxide building block,the chirality from anhydride and the configurational match with epoxide remain elusive.Herein,we discover that the bimetallic chromium catalysts have led to an obvious enhancement in terms of reactivity and enantioselectivity for the asymmetric copolymerization of meso-epoxide with various non-symmetric chiral anhydrides.Up to 97%ee was obtained during the asymmetric copolymerization of cyclohexene oxide(CHO)with(R)-methylsuccinic anhydride(R-MSA),and three-or four-carbon chiral centers were simultaneously installed in the aliphatic polyester backbone.In particular,the different combinations of stereochemistry in epoxide and anhydride building blocks considerably affect the thermal properties and crystalline behaviors of the resulting polyesters.This study uncovers an interesting method for regulating polymer crystallinity via matching the chirality of different monomers.
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).
